REVIEW

pubs.acs.org/IECR

Rice Husk and Its Ash as Low-Cost Adsorbents in Water and

Wastewater Treatment
M. Ahmaruzzaman*,† and Vinod K. Gupta‡,§
†
Department of Chemistry, National Institute of Technology Silchar, Silchar-788010, Assam
‡
Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee-247667, Uttarakhand
§
Chemistry Department, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia

ABSTRACT: Rice husk, which is a relatively abundant and inexpensive material, is currently being investigated as an adsorbent for
the removal of various pollutants from water and wastewaters. Various pollutants, such as dyes, phenols, organic compounds,
pesticides, inorganic anions, and heavy metals can be removed very effectively with rice husk as an adsorbent. This article presents a
brief review on the role of rice husk and rice husk ash in the removal of various pollutants from wastewater. Studies on the adsorption
of various pollutants by rice husk materials are reviewed and the adsorption mechanism, influencing factors, favorable conditions,
etc., discussed in this article. It is evident from the review that rice husk and its ash can be potentially utilized for the removal of
various pollutants from water and wastewaters.

1. INTRODUCTION Dyes are widely utilized in industries such as textiles, rubber,

Environmental pollution has reached a stage in which it should
be seriously examined; otherwise, civilization will be in real
danger. Among the various types of pollution, water pollution
has attracted the attention of various researchers and scientists
around the world. The problem of removing various pollutants
from water and wastewater has grown with rapid industrializa-
tion. Heavy metals, dyes, phenols (including other organic
compounds), inorganic anions, and pesticides (which are toxic
to many living lifeforms and organisms) are present in the
wastewater streams of many industrial processes. Dyeing, print-
ing, mining and metallurgical engineering, electroplating, nuclear
power operations, semiconductor, aerospace, and battery man-
ufacturing processes are some of the industries that are
generating various types of pollutants in the wastewater
effluents.1,2 All of the above-mentioned industries are faced
with increasing pressure, regarding environmental and waste-
related concerns, as a result of the quantity and toxicity of the
wastewaters generated. There are several methods available
for the removal of dyes, organic pollutants, pesticides, heavy
metals, and other industrial effluents from wastewaters
(including membrane filtration, coagulation, adsorption, oxi-
dation, ion exchange, and precipitation). However, some of
them were utilized because of their low cost, high efficiency,
and applicability to a wide variety of pollutants. Heavy-metal
contamination exists in aqueous waste streams from many
industries, such as metal plating, mining, tanneries, painting,
and car radiator manufacturing, as well as agricultural sources,
where fertilizer and fungicidal spray are intensively used.
Metals such as copper, zinc, chromium, and cadmium are
harmful wastes that are produced by industry and pose a risk
of contaminating groundwater and other water resources.
Heavy metals are not biodegradable and tend to accumulate
in living organisms, causing various diseases and disorders. For
example, chromium causes serious ailments in both animal and
plant bodies.3
paper, plastics, and cosmetics, to impart color of their products.
The dyes are invariably left as the major waste in these industries.
Many of the organic dyes are hazardous and may affect aquatic
life and even the food chain. For example, Malachite Green,
which is a common silk and cotton dyeing agent, has been found
to be highly cytotoxic in mammalian cells and also acts as a
liver tumor-enhancing agent. Therefore, the removal of dyes is
essential for the protection of the environment.4
In developed countries such as the United Kingdom (U.K.)
and many European Union (EU) countries, environmental
policies have required that zero synthetic chemicals should be
released into the marine environment.5 Because of their chemical
structures, dyes are resistant to fading upon exposure to light,
water, and many chemicals; therefore, these compounds are
difficult to decolorize once they are released into the aquatic
environment.6,7 Treatment processes for metal-contaminated
waste streams include chemical precipitation, membrane filtra-
tion, ion exchange, carbon adsorption, and coprecipitation/
adsorption.8 These processes usually require expensive facilities
and have high maintenance costs. More economical alternative
technologies or sorbents for the treatment of metal-contaminated
waste streams are needed.
Increasing use of pesticides in agriculture, forestry, and
domestic activities for controlling pests is polluting our water
resources day by day. The leaching runoff from agricultural and
forest lands; deposition from aerial applications and discharge of
industrial wastewater are responsible for this water contamina-
tion. The pesticides form a strong class of water pollutants,
because they are sometimes nonbiodegradable. Moreover, pes-
ticides are carcinogenic in nature. Therefore, the toxicity of
Received: July 11, 2011
Accepted: October 28, 2011
Revised: October 9, 2011
Published: October 28, 2011

r 2011 American Chemical Society 13589 dx.doi.org/10.1021/ie201477c | Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

Table 1. Permissible Limits and Health Effects of Various Toxic Heavy Metalsa

Permissible Limits for Industrial

Effluent Discharge (mg/L)

Permissible Limits for

Indian Standard WHO Potable Water (mg/L)

inland public marine inland Indian standard

metal surface water sewers coastal areas surface water IS 10500 WHO USEPA EU Standard health hazards

nickel 3.0 3.0 5.0 0.02 0.02 0.1 0.02 causes chronic bronchitis, reduced lung function,
cancer of the lungs
zinc 5.0 15.0 15.0 5.0
15.0 5.0 3.0 5.0 causes short-term illness called “metal fume fever”
and restlessness
copper 3.0 3.0 3.0 0.05
1.5 1.5 2.0 1.3 2.0 long-term exposure causes stomach ache, irritation
of nose, mouth, and eyes, headaches
cadmium 2.0 1.0 2.0 0.1 0.01 0.003 0.005 0.005 carcinogenic, causes lung fibrosis, dyspnoea
lead 0.10 1.0 2.0 0.1 0.05 0.01 0.015 0.01 suspected carcinogen, anemia,
muscle and joint pains,
kidney problems, and high blood pressure
total chromium 2.0 2.0 2.0 0.05 0.05 0.1 0.05 suspected human carcinogen,
producing lung tumors
arsenic 0.2 0.2 0.2 0.01 0.01 0.01 0.01 carcinogenic, producing liver tumors, and
gastrointestinal effects
mercury 0.01 0.01 0.01 0.001 0.001 0.002 0.001 excess dose may cause headache, abdominal pain,
and diarrhea, paralysis, and gum inflammation,
loosening of teeth, loss of appetite, etc.
iron 3.0 3.0 3.0 0.1
1.0 0.3 0.2 0.3 0.2 excess amounts cause rapid pulse rates, congestion
of blood vessels, hypertension
manganese 2.0 2.0 2.0 0.05
0.5 0.1 0.5 0.05 0.05 excess amounts toxic, and causes growth
retardation, fever, sexual impotence,
muscles fatigue, eye blindness
vanadium 0.2 0.2 0.2 1.4 very toxic, and may cause paralysis
a
Data taken from ref 11.

pesticides and their degradation products makes these chemical
substances a potential hazard by contaminating our environment.
Phenols are generally considered as one of the important
organic pollutants discharged into the environment; such com-
pounds give an unpleasant taste and odor to drinking water. The
major sources of phenol pollution in the aquatic environment are
wastewaters from paint, pesticide, coal conversion, polymeric
resin, and the petroleum and petrochemicals industries. Introduc-
ing phenolic compounds into the environment or degradation
of these substances means the appearance of phenol and its
derivatives into the environment. The chlorination of natural
waters for disinfection produces chlorinated phenols. Phenols
and other phenolic compounds are considered as priority pollutants,
because they are harmful to organisms at low concentrations.9,10
Adsorption with activated carbon was highly efficient for the
removal of various impurities/pollutants from wastewater; how-
ever, the high cost of activated carbon inhibits its large-scale
application as an adsorbent. Therefore, there is a need for the
effective removal of various pollutants from wastewaters and
resulted in a search for various low-cost adsorbents utilized for
the removal of various impurities, such as heavy metals, dyes,
pesticides, and other organic pollutants.1
4 Table 1 shows the per-
missible limits and health effects of various toxic heavy metals.11
The permissible limits and health effects of various inorganic
13590
anions, pesticides and other organic compounds are also shown
in Tables 2 and 3.12
14
Natural materials that are available in large quantities, or
certain waste products from industrial or agricultural operations,
may have potential as inexpensive adsorbents. The abundance,
availability, and low cost of agricultural byproducts make them
good adsorbents for the removal of various pollutants from
wastewaters. Agricultural waste biomass currently is gaining
importance. In this perspective rice husk, which is an agro-based
waste, has emerged as an invaluable source for the utilization in
the wastewater treatment. Rice husk contains ∼20% silica, and it
has been reported as a good adsorbent for the removal of heavy
metals, phenols, pesticides, and dyes. Rice husk is extensively
used in rural India, because of its widespread availability and
relatively low cost. The annual generation of rice husk in India is
∼18
22 million tons.15 These rice husks, as a commodity waste,
can also be made into activated carbon, which is used as an
adsorbent in the wastewater treatment. It would add value to
these agricultural commodities, help to reduce the cost of waste dis-
posal, and provide a potentially inexpensive alternative to the
existing commercially available activated carbons. Rice husks are
accounting for approximately one-fifth of the annual gross of rice in
the world (545 million metric tons).16 Because of the growing
concern with environment pollution, and the need to conserve
dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

Table 2. Permissible Limits and Health Effects of Various Organic Compounds, Pesticides, and Inorganic Anionsa

Permissible Limits for Industrial

Effluent Discharge (mg/L)

Indian Standard

compound inland surface water public sewers marine coastal areas health hazards

phenols 1.0 5.0 5.0 headache; fainting; vertigo; mental disturbances; ochronosis; vomiting;
difficulty swallowing; ptyalism; diarrhea; and anorexia
oil and grease 10.0 20.0 10.0
pesticides 0.010 0.010 0.010 highly poisonous to humans and animals; destruction of nerve
cells in certain regions of brain, resulting in a loss of dopamine
benzene hexachloride 0.010 0.010 0.010 carcinogenic; nausea; eye irritation; headache;
shallow breathing; endocrine disrupter
DDT 0.010 0.010 0.010 affects stomach, intestines, heart, blood vessels, kidneys, and
nervous system; kidney and liver dysfunction; breast cancer;
Hodgkin’s disease; skin, lung, and liver cancer; general weakening
of the immune system, lymphatic system, and reproductive system
endosulfun 0.010 0.010 0.010 itching; burning; tingling of the skin; headache; dizziness; nausea;
vomiting; lack of coordination; tremor, mental confusion
seizures, respiratory depression, coma
malathion 0.010 0.010 0.010 headache; excessive salivation and tearing; muscle twitching; nausea;
diarrhea; respiratory depression; seizures; loss
of consciousness; pinpoint pupils
methyl malathion 0.010 0.010 0.010 headache; excessive salivation and tearing, muscle twitching; nausea;
diarrhea; respiratory depression; seizures;
loss of consciousness; pinpoint pupils
paraquat 2.30 2.30 2.30 burning in mouth, throat, chest, and upper abdomen; diarrhea;
giddiness; headache; fever, lethargy; dry,
cracked hands; ulceration of the skin
cyanides 0.20 2.00 0.20 very poisonous; affects brain and heart and leads to coma and death
fluorides 2.00 15.00 15.00 dental fluorosis; bone cancer; affects CNS
boron 2.00 2.00 2.00 irritation of eye, upper respiratory tract, and nasopharynx
phosphate 5.0
a
Data taken from ref 12.

energy and resources, efforts have been made to burn rice husks
under controlled temperature and atmosphere as supplementary
cementing material. However, the amount of rice husk available is
far in excess of any local uses and, thus, has posed disposal
problems. Rice husk was chosen to be applied as a precursor
material, because of its granular structure, insolubility in water,
chemical stability, high mechanical strength, and its local availability
at almost no cost. The advantage in the application of rice husk and
its ash as adsorbents is that there is no need to regenerate them,
because of their low production costs.
The utilization of rice husk would solve both a disposal
problem and also access to less-expensive material in the waste-
water treatment. It has the potential to be used as an adsorbent,
because of the presence of carbon and silica. When rice husk is
burnt, ∼20 wt % of the ash is generated. The rice husk ash
(RHA) has more than 95 wt % of silica with high porosity and
large surface area, because it retains a cellular structure skeleton.
An overview of rice husk and RHA as low-cost adsorbents is
presented in this paper, and their removal performance is
compared. The main goal of this review is to provide a summary
of information concerning the utilization of rice husk and RHA
as adsorbents for the removal of heavy metals, dyes, organic
13591
compounds, surfactants, pesticides, and inorganic anions from
wastewater. It also highlights that chemically modified rice husk
has enhanced adsorption capacities for heavy metals, phenols,
pesticides, dyes, and other organic compounds from wastewaters.
2. PROPERTIES OF RICE HUSK AND RICE HUSK ASH
Rice husk possesses a granular structure, is insoluble in water,
and has chemical stability and high mechanical strength, making
it a good adsorbent material for treating various wastes from
water and wastewater. Tables 4 and 5 show the physico-
chemical properties and chemical compositions of rice husk,
respectively,17
26 whereas the properties of rice husk ash
(RHA) are shown in Tables 6 and 7.21,23,27
30 The chemical
components of RHA are found to be SiO2, H2O, Al2O3, Fe2O3,
K2O, Na2O, CaO, and MgO (Table 6), fluctuating upon the
varieties of paddy, proportion of irrigated area, geographical con-
ditions, fertilizer used, climatic variation, soil chemistry, and time-
liness of crop production operations and agronomic practices in
the paddy growth process.31,32 From chemical analysis via energy-
dispersive X-ray spectroscopy (EDX), it is indicated that the most
abundant component in rice husk is silicon. The morphology of
dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

Table 3. Permissible Limits and Health Effects of Various Organic Compounds and Inorganic Anionsa

Permissible Limits for Potable Water (mg/L)

species Indian Standard WHO (μg/L) USEPA EU Standard health hazards

phenols 0.001
polychlorinated biphenyls 0.0005 0.0005 skin changes; thymus gland problems; immune deficiencies;
reproductive or nervous system difficulties; increased risk of cancer
pentachlorophenols 0.009 0.001 0.0001 liver or kidney problems; increased cancer risk
benzene 0.01 0.005 0.001 carcinogen; dizziness; sleepiness; convulsions; and death
toluene 0.7 1.0 carcinogen; liver and kidney damage; memory loss; and death
xylenes 0.5 10 carcinogen; dizziness; headache; affects stomach,
CNS, liver, and kidneys
ethyl benzenes 0.3 0.7 affects eyes and respiratory tract; irritation of throat, eyes, and nose
styrene 20 0.1 possible carcinogen; affects CNS; irritations
of respiratory tract, skin, and eyes
polynuclear aromatic 0.0001 0.7 0.0002 carcinogen; affects gastrointestinal, renal, and pulmonary system
hydrocarbons (PAH)
monochlorobenzene 0.3 0.1 irritation; vomiting; diarrhea; nausea; headaches; sleepiness;
dichlorobenzene also affects central nervous system, respiratory tract.
trichlorobenzene 200 0.07 itching, pain, and eye damage, etc.
carbofuran 0.007 0.04 0.0001 affects blood, reproductive, and nervous systems
lindane 0.0002 0.0002 affects nervous system, liver and kidneys, and may be a carcinogen
alachlor 0.02 0.002 0.002 anemia, possible carcinogen, and also affects liver, kidneys, and eyes
benzo [α] pyrene 0.0007 0.0002 0.00001 carcinogen; toxicity in bone marrow and reproductive system
atrazine 0.002 0.002 0.003 0.0001 irritating to skin, eyes, and respiratory tract;
abdominal pain; diarrhea; vomiting
paraquat 0.0001
fluoride 1.0 1.5 4.0 1.5
nitrate 45 11 10 11 methemoglobinemia; stomach acidity
boron 1 0.5 1
bromate 0.01 0.01 0.01 nausea; vomiting; diarrhea and abdominal pain; affects kidney, CNS
cyanide 0.05 0.07 0.2 0.05
a
Data taken from refs 13 and 14.

Table 4. Proximate and Ultimate Analyses of Rice Huska

Proximate Analysis (wt %) Ultimate Analysis (wt %)

combustibles moisture ash voltaile matter fixed carbon C H O N S Cl

72.87 10.00 17.13 38.92 5.55 37.94 0.35 0.02 0.09

19.8 64.3 15.9 37.00 5.10 36.00 0.40
7.9 17.1 59.9 44.6 5.6 49.3
20.00 66.40 13.60 37.8 5.20 39.0 0.39 0.05
17.9 72.8 9.3 48.9 6.2 44.1 0.8
a
Data taken from refs 17
22.

rice husk may facilitate the adsorption of metals and other
pollutants, because of the irregular surface of rice, thus making
possible the adsorption of metals in different parts of this material.
The physical characterizations of rice husk and RHA have pointed
out some properties such as the presence of functional groups
(carboxyl, silanol, etc.) that make adsorption processes possible.
The chemical structure of the rice husk is of vital importance in
understanding the adsorption process. The Fourier transform
infrared (FTIR) technique is an important tool to identify the
characteristic functional groups, which are instrumental in the
adsorption of various pollutants from water and wastewaters.
13592
To get better insight into the surface functional groups present
on the surface of rice husk, FTIR spectra of rice husk, RHA, and
metal-loaded RHA are presented in Figures 1 and 2, respec-
tively.34 Table 8 also highlights the major stretching frequencies
of the surface functional groups present in rice husk and its ash.
The spectra shows that silanol groups may be present in the
form of a silicon dioxide structure (
Si
O
Si
OH) and is
similar to the silanol groups of silicic acid.38 The presence of
polar groups on the surface is likely to give considerable cation
exchange capacity to the adsorbents. 39 With the loading of
metal ions, the shifting of the peaks is found from ∼3430, 2920,
dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

Table 5. Chemical Analysis of the Rice Huska

composition (%)

cellulose 32.24 34.4 29.20 32.24 33.47

hemicellulose 21.34 29.3 20.10 21.34 21.03
lignin 21.44 19.2 30.70 21.44 26.70
extractives 1.82 1.82
water 8.11 8.11
mineral ash 15.05 17.1 15.05 Figure 1. Fourier transform infrared (FTIR) spectra of rice husk.
a
Data taken from refs 18, 19, and 23
26. (Adopted with permission from ref 21. Copyright 2003, Elsevier.)

Table 6. Chemical Composition of Rice Husk Asha

constituent (%)

SiO2 94.50 92.00 94.64 88.47 81.09 92.40

Al2O3 0.29 0.05 0.30
Fe2O3 <0.50 0.1 0.23 0.40 0.14 0.40
CaO 0.25 1.28 1.89 1.80 1.07 0.70
MgO 0.23 0.37 0.96 0.71 0.75 0.30
Na2O 0.78 0.05 0.39 0.26 0.07
K2O 1.18 2.19 0.58 2.50 1.39 2.54
SO3 0.6 0.94 1.45
loss on ignition, LOI 3.43 8.73 2.31
Zn (ppm) 18.20 32.28
Mn (ppm) 52.24 56.44
Cu (ppm) 32.17 16.98
Cd (ppm) 0.48 0.49
a
Data taken from refs 21, 23, and 27
29. Figure 2. FTIR spectroscopy of rice husk ash (RHA) (spectrum 1) and
metal-ion-loaded RHA specimens (RHA-Cd (spectrum 2), RHA-Ni
(spectrum 3), and RHA-Zn (spectrum 4)). (Adopted with permission
Table 7. Characteristics of Rice Husk Asha from ref 34. Copyright 2006, Elsevier.)
parameter value is visible. These characteristics indicate that
CO
,
OH,
average particle size 412 μm
Si
OH,
Si
H, and
C
OH groups are effective in the
bulk density 175.3 kg m
3 adsorption of Cd(II), Ni(II) and Zn(II) onto RHA.34
moisture content 1.1%
The morphological studies of rice husk and RHA are shown in
Figures 3 and 4, respectively.40,41 Typically, rice husk has a
volatile matter content 7.36%
globular structure in nature, of which its main components are in
ash content 80.58%
the lemma or palea form, tightly interlocked with each other.42
fixed carbon content 10.96% The corrugate structural outer epidermis is highly ridged, con-
heating value 21.76 MJ kg
1 taining papillae and hairs of varying sizes and well-organized in a
BET surface area 65.36 m2 g
1 linear profile (linear ridges and furrows), while its ridges are
BJH adsorption surface area of pores 52.35 m2 g
1 punctuated with the prominent globular protrusions.40 However,
BJH desorption surface area of pores 26.62 m2 g
1 the biomass are assembled around the stable Si
O carcass,
cumulative pore volume 0.039 cm3 g
1 concentrated in the protuberances and hairs (trichomes) on
BET pore diameter 34.66 Å the outer and inner epidermis, adjacent to the rice kernel.43 Many
BJH adsorption average pore diameter 43.27 Å cavities having varying particle sizes were distributed within the
BJH desorption average pore diameter 58.34 Å
ash samples, as evidenced of the interconnected porous network
a and large internal specific surface area.44 Figure 5 showed the
Data taken from ref 30.
X-ray diffraction (XRD) analysis of RHA and indicated that
quartz is the only crystalline phase present in the ash.45 It is
1636, 1092, 792, and 468 cm
1 and the shifting occurs both to reported that the halo centered at 2θ ≈ 20° corresponds to black
higher and lower wavenumbers. This indicates that the functional calcinated amorphous organic matter or amorphous silica.
groups at these wavenumbers participated in the adsorption of
metals. The FTIR spectra for cadmium-loaded RHA (RHA-Cd)
shows the disappearance of bands ∼2900 and 1636 cm
1, and 3. COMPETING TECHNOLOGIES AVAILABLE FOR THE
shifting of bands ∼1092, 792, and 468 cm
1 to lower wave- REMOVAL OF HEAVY METALS, DYES, PESTICIDES, AND
numbers.34 Such a disappearance of bands is not observed in OTHER ORGANIC POLLUTANTS FROM WASTEWATERS
the case of Ni- and Zn-loaded RHA (RHA-Ni and RHA-Zn, Treatment processes for metals, phenols, dyes, and pesticides
respectively) spectra, although the shifting of all the bands contaminated wastewaters include chemical precipitation,
13593 dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

Table 8. Surface Functional Groups Present in the Rice Husk

and Rice Husk Asha
wavelength (cm
1) groups present

3400 surface hydroxyl groups and

chemisorbed water33
2800 and 3700, free and hydrogen bonded OH
with a small band groups and Si
OH group
at ∼3400 and ∼2920 on the surface of rice husk ash
(RHA), because of presence of
both the silanol groups (Si
OH)
and adsorbed water (peak at 3430 cm
1)
Figure 4. SEM micrographs of rice husk ash (RHA). (Adopted with
on the surface35
permission from ref 41. Copyright 2008, Elsevier.) (Bar = 20 μm.)
2940 and 2820 stretching of OH groups bound
to methyl radicals
1740 and 1662 ketonic and aldehydic CdO stretching
frequencies
1600
CO and
C
OH groups stretching
from aldehydes and ketones
1470 and 1380
CH2 and
CH3 groups
1465 and 1400 C
O stretching vibration of
carboxylate groups36
1300 aromatic CH and carboxyl-carbonate
structures and silanol groups37
1050
1300 vibration of the CO group in lactones
1100 Si
O
Si and
C
O
H stretching
and
OH deformation
1080 Si
O
Si bond Figure 5. X-ray diffraction (XRD) analysis of the RHA. (Adopted with
793 and 469 Si
H permission from ref 45. Copyright 2000, Elsevier.)
460 metal
halogen bond
a used for the treatment of wastewaters, along with their advantages
Data taken from refs 33
37.
and disadvantages.46
Reverse osmosis is a process where polluted water is forced to
pass through a semipermeable membrane that allows only water
to pass but not the pollutants; this membrane is also expensive.
Electrodialysis separates ionic components through semiperme-
able ion-selective membranes. The main disadvantage of this
method is the formation of metal hydroxides, which clog the
membrane. Ultrafiltration utilizes pressure-driven membrane
filtration for the removal of pollutants; however, the generation
of sludge is a problem.
Ion exchange is often the method of choice, especially in the
nuclear industry; it invovles the exchange of metal/radionuclide
species from dilute solutions with ions held by electrostatic forces
on a suitable ion-exchange resin. Some disadvantages include
high cost and the only partial removal of certain ions. However,
unlike biomass-based adsorption systems, they have the capacity
to be highly selective. Chemical precipitation is achieved by the
addition of coagulants such as alum, lime, iron salts, and other
Figure 3. Scanning electron microscopy (SEM) micrographs of rice organic polymers, with a large amount of sludge being produced
husk (RH), showing the protuberance, outer epidermis, and silica content. that contains toxic compounds. Solvent (or liquid) extraction
(Adopted with permission from ref 40. Copyright 2003, Elsevier.) (Bar =
100 μm.)
depends upon the selective dissolving of one or more constitu-
ents of the contaminated solution into a suitable immiscible
liquid solvent. The simplest and least-expensive method of
oxidation/reduction, reverse osmosis, solvents extraction, co- removing most metals from solution is to increase the pH,
agulation, electrochemical, irradiation, photochemical, ozonation, converting the soluble metal into an insoluble form (i.e., hydrox-
membrane filtration, ion exchange, and adsorption. All the above ide). However, precipitation by adjusting the pH is not selective
processes have their disadvantages and advantages. The major and precipitation by alkali addition (usually lime) produces large
methods of industrial wastewater treatment involve physical and/ quantities of solid sludge for disposal. However, precipitation
or chemical processes. Table 9 summarizes the various processes processes can be highly efficient. The type of process utilized will
13594 dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research
Table 9. Current Treatment Technologies for the Removal of Various Pollutants, Involving Physical and/or Chemical Processesa
physical and/or chemical methods advantages
oxidation rapid process for toxic pollutants removal
ion exchange good removal of a wide range of heavy metals
membrane filtration technologies good removal of heavy metals
adsorption flexibility and simplicity of design, ease of
operation and insensitivity to toxic pollutants
coagulation/flocculation economically feasible
electrochemical treatment rapid process and effective for certain metal ions
ozonation applied in gaseous state: alteration of volume
photochemical no sludge production
irradiation effective at lab scale
electrokinetic coagulation economically feasible
Fenton’s reagents effective and capable of treating variety of wastes and
no energy input necessary to activate hydrogen peroxide
biological treatment feasible in removing some metals
a
Data taken from ref 46.
be dependent on the substances to be treated and the target
effluent concentrations. Overall process costs, both operational and
capital, will be influenced by several criteria, such as versatility
and simplicity. Adsorption process is efficient for the removal of
various impurities/contaminants from water as well as wastewaters.
Activated carbons are the widely used adsorbents, because of
their good adsorption abilities for various pollutants present in
wastewaters. The high initial cost of activated carbon and the need
for a costly regeneration system make it less economically viable
as an adsorbent. Therefore, many researchers have investigated
various agricultural waste materials, such as rice husk and ash as
adsorbents for the removal of impurities/contaminants from
water and wastewaters.
4. RICE HUSK AS AN ADSORBENT FOR THE REMOVAL
OF HEAVY METALS
4.1. Heavy Metals Removal by Natural Rice Husk. Rice husk
(RH) has been intensively investigated as an adsorbent for the
removal of heavy metals from wastewaters. Table 10 summarizes
the adsorption capacity of the metal ions investigated on RH and
ash. The potential of RH for the removal of heavy metals from
aqueous solution was reviewed and reported that the most
investigated metals included Cd, Pb, Zn, Cu, Co, Ni, and Au.47
Sumathi et al.48 investigated RH for their effectiveness in
removing chromium from tannery effluent through batch experi-
ments and compared the adsorption capacity of RH with
sawdust, coir pith, and charcoal. The sawdust exhibited a higher
adsorption capacity, followed by coir pith. RH was utilized for the
removal of lead(II) from aqueous solution49 and reported that
the pH of aqueous solution affected the removal of lead(II) and
removal efficiency increased with increased solution pH. The
maximum adsorption was ∼87.75% at a pH of 4.6 ( 0.5, and an
initial concentration of 30 mg/L.
The effects of initial concentration of lead, temperature, rice
husk loading, and pH were investigated for an optimized condi-
tion of lead uptake from the aqueous solution.50 The optimization
process was analyzed using Central Composite Face-Centered
Experimental Design in Response Surface Methodology (RSM)
by Design Expert Version 5.0.7. Under the optimum conditions,
the lead uptake was reported to be 8.60 mg/g.
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REVIEW
disadvantages
high energy costs and formation of byproduct
absorbent requires regeneration or disposal
concentrated sludge production, expensive
adsorbents requires regeneration
high sludge production and formation of large particles
high energy costs and formation of byproduct
short half-life
formation of byproduct
requires a lot of dissolved O2
high sludge production
sludge generation
technology yet to be established and commercialized
The potential of rice husk was also assessed for the adsorption
of nickel from aqueous solutions.51 The efficiency of rice husk for
nickel removal was 51.8% for dilute solutions at an adsorbent
dose of 20 g/L. FTIR, SEM, and EDAX were investigated before
and after adsorption to explore the number and position of the
functional groups available for nickel binding on the rice husk
and changes in surface morphology and elemental constitution of
rice husk.51 The removal of poisonous lead(II) from wastewater
by rice husk was investigated by Abdel-Ghani et al.52 The
adsorption capacity of rice husk was compared to that of maize
cobs and sawdust. The adsorption efficiencies were reported to
be pH dependent, increased with increased solution pH from 2.5
to 6.5. Rice husk was also utilized for the removal of arsenic from
water and wastewaters.53 Maximum adsorption was reported at
0.01 mol/L of HNO3, HCl, H2SO4, or HClO4 using 1.0 g of
adsorbent for 5.97  10
3 mol/L of arsenic for 5 min and the
uptake of arsenic increased with increased temperature.
Amin et al.54 also utilized rice husk for aqueous arsenic
remediation. Complete removal of both As(III) and As(V) was
achieved under the following conditions: initial As concentra-
tion, 100 μg/L; rice husk amount, 6 g; average particle size, 780
and 510 μm; flow rate, 6.7 and 1.7 mL/min; and pH, 6.5 and 6.0,
respectively. Desorption (71%
96%) was also achieved with 1 M
of KOH.
Rice husk was tested for the adsorption of Zn(II) and Pb(II)
ions from dairy wastewater.55 The percent adsorption of Zn(II)
and Pb(II) ions increased with increased contact time and dosage
of rice husk. The binding process was strongly affected by pH and
the optimum pH for Zn(II) and Pb(II) ions were 7.0 and 9.0,
respectively. The maximum adsorption capacities for Zn(II) and
Pb(II) ions were reported as 19.617 and 0.6216 mg/g, respec-
tively. Roy et al.56 investigated the potential of rice husk for the
adsorption of arsenic, cadmium, chromium, lead, and strontium
from wastewaters. The rate of adsorption was fast; the solution
metal concentration reached equilibrium within minutes. The
cell wall metal complex was found to be stable; the bound metal
did not desorb over time under static conditions. Most of the
cationic metal ions were recovered from the rice husk through
desorption by lowering the pH of the medium.
The ability of rice husk to remove chromium, zinc, copper, and
cadmium from wastewater has been investigated.57 Under the
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Industrial & Engineering Chemistry Research REVIEW

Table 10. Maximum Heavy Metals Adsorption Capacities for Table 10. Continued
Rice Husk and Rice Husk Ash adsorbent adsorption capacity (mg/g) reference
adsorbent adsorption capacity (mg/g) reference 45 68
5.69 50
Zn(II) Metal 58.1 74
rice husk ash 5.88 141 0.6216 55
3.08 142 tartaric acid
RH 108 71
14.30 59
Hg(II) Metal
26.10 78
rice husk ash 9.32 70
9.588 82
46.14 75
17.84 77
rice husk 66.66 75
rice husk 0.75 67
29.69 64 As(III) Metal
0.17 57 activated rice husk 1.22 120
19.617 55
Ni(II) Metal optimal conditions, removal of the Cr, Zn, Cu, and Cd ions from
rice husk ash 4.71 140 aqueous solution are 79%, 85%, 80%, and 85%, respectively, and
2.62 142 hydrochloric acid (HCl) solution was utilized for the recovery
25.33 78 of adsorbed metals from rice husk. The removal of Cr(VI) from
13.89 77 aqueous solution onto rice husk was also reported.58 The authors
rice husk 0.23 67
compared the adsorption studies with other adsorbents such as
clarified sludge (a steel industry waste material), activated
5.52 74
alumina, fuller’s earth, fly ash, saw dust, and neem bark. Adsorp-
8.86 51
tion process was highly pH-dependent and optimum pH range
Cd(II) Metal for adsorption of Cr(VI) was reported between 2 and 3. The
rice husk ash 3.04 140 adsorption capacity (qmax) and the Gibbs free energy (ΔG°)
2.30 142 value indicated that clarified sludge was the most effective among
25.27 78
the studied adsorbents for the removal of Cr(VI) from aqueous
solution. The adsorption efficiencies of rice husk ash (RHA) and
11.79 77
activated alumina were also equally comparable to that of clarified
rice husk 21.36 56
sludge. The same research groups59 have extended their work on
0.16 57 the removal of Zn(II) from aqueous solution onto rice husk.
4.0 68 Rice husk in natural form and activated carbon from rice husk
8.82 69 was utilized for the removal of chromium(VI) and results were
16.7 74 compared with commercial activated carbon.60,61 Rice husk and
HNO3-treated rice husk 11.03 69 water hyacinth along with other low-cost adsorbents were studied
26.31 58 for the removal of arsenic and the efficiency varies between 71%
rice husk 164.31 56 and 96%.62 Rice husk was selected for adsorption of gold
thiourea
4.02 57 complex and compared with activated carbon.63 The maximum
14.2
31.5 3
gold adsorption of heated rice husk, and activated carbon was
28.22 and 35.88 mg Au/g adsorbent, respectively. FTIR spec-
activated rice husk 45.6 61
trum, thermodynamic study, and elution studies indicated that
Cu(II) Metal heated rice husk adsorbed gold by chemical adsorption. The
rice husk 1.21 67 active functional groups of heated rice husk were ketone,
0.2 57 carboxylate, and siloxane, as suggested by the authors.63 Gold
29 71 adsorbed onto heated rice husk, and activated carbon was
31.85 71
reported to be eluted by 0.5 M Na2S2O3 to 87 and 41%,
respectively. The authors recommended that heated rice husk
2.48 69
could be used as an alternative adsorbent for gold
thiourea
HNO3-treated rice husk 9.36 69 preconcentration.
activated rice husk 112.43 145 Most of the reported heavy-metal adsorption studies sug-
tartaric acid
RH 29 71 gested the applicability of Langmuir isotherm, which assumes
Pb(II) Metal monolayer coverage and constant adsorption energy on the
surface of the adsorbent. However, some studies reported that
rice husk ash 12.63 76
the adsorption data of Zn(II) on rice husk are well-fitted to the
91.74 81
Freundlich isotherm, rather than the Langmuir isotherm.64
207.50 80 4.2. Heavy Metals Removal by Modified Rice Husk. It is
rice husk 11.40 56 evident from the literature that modified/treated rice husk
108 71 possessed a better adsorption capacity for the removal of heavy
129.48 71 metals than natural rice husk. Various methods/techniques were
13596 dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research
utilized by the researchers for the modification of rice husk. As
mentioned in Table 5, rice husk consists of cellulose, hemicellu-
loses, lignin, and mineral ash, and there is a high percentage of
silica in its mineral ash. Pretreatment of the rice husk can remove
lignin and hemicellulose, reduce cellulose crystallinity, and
increase the porosity or surface area. In general, chemically
modified or treated rice husk exhibited higher adsorption capac-
ities on heavy metal ions than nonmodified rice husk. Suemitsu
et al.65 reported that better adsorption capacity on metal ions was
achieved with treated rice husk. They have utilized Procion Red-
and Procion Yellow-treated rice husk for the removal of Cr(VI),
Ni(II), Cu(II), Zn(II), Cd(II), Hg(II) and Pb(II) ions from
aqueous solution. The percentage removal of Cd(II), Pb(II) and
Hg(II) ions were reported to be more than 80% by these two
types of treated adsorbents, while Cr(VI) showed the lowest
percentage removal (<40%). Activated rice husk (ARH) was also
investigated for the removal of heavy metals, such as Zn(II),
Cu(II), and Cr(VI) from textile dye effluent.66 Removal of heavy
metal ions from the textile dye effluent increased with increased
adsorbent dosage. In ARH, at 50 g/L, the maximum removals of
62%, 68%, and 65% of Zn(II), Cu(II), and Cr(VI), respectively,
are obtained. Ion exchange is reported to be the major mecha-
nism for the removal of metal ions by ARH.
Marshall et al.67 reported that better adsorption capacity on
metal ions was achieved with modified rice husk; they also
reported that the method of treatment affects the adsorption
capacities. Modified rice husks treated with NaOH were reported
to have a higher adsorption capacity for Pb(II) and Cd(II),
compared to that of nonmodified rice husk.68 Ong et al.69
investigated the adsorption behavior of Cu(II) and Cd(II) ions
onto modified rice husk and observed that the adsorption
capacity of rice husk increased after treatment with nitric acid.
The properties of rice husk were reported to vary with the
method of modification and strongly influenced the adsorption
capacity.47 Feng et al.70 observed that rice husk heated at high
temperature (700 °C) increased the specific surface area and
increased the adsorption capacity of lead and mercury from
aqueous solution. Rice husk was modified by various types of
carboxylic acids (citric acid, salicylic acid, tartaric acid, oxalic acid,
mandelic acid, malic acid, and nitrilotriacetic acid) and reported
that tartaric acid-modified rice husk exhibited the highest ad-
sorption capacities for the removal of copper and lead from
aqueous solutions.71 The carboxyl groups on the surface of the
modified rice husk were primarily responsible for the adsorption
of metal ions. Adsorption kinetics suggested that the rate-limiting
step may be chemical adsorption, rather than diffusion. The
presence of chelators on the uptake of lead by tartaric acid-
modified rice husk was also investigated by the same authors and
reported that higher molar ratios of chelators such as nitrilotria-
cetic acid (NTA) and ethylenediamine tetraacetic acid (EDTA)
caused a significant suppressing effect on the adsorption of lead.
Ajmal et al.72 showed that adsorption of Ni(II) and Cd(II) was
higher when phosphate-treated rice husk was used, compared to
that of raw rice husk. It was also observed that recovery of Cd(II)
from synthetic wastewater by column operation was better than a
batch process. Rice husk is also tested for the removal of Cd(II)
from aqueous solution, and chemical modifications increased the
adsorption capacity of rice husk.73 The adsorption capacity of
rice husk increased from 8.58 mg/g to 11.12, 20.24, and 16.18
mg/g and the equilibrium time decreased from 10 h for rice husk
to 2, 4, and 1 h for epichlorohydrin-, NaOH-, and NaHCO3-
treated rice husks, respectively. The equilibrium data was
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REVIEW
reported to follow a pseudo-second-order kinetics model, which
agreed with chemisorption as the rate-limiting mechanism.
A biomatrix was prepared from rice husk for the removal of several
heavy metals from their aqueous solutions.74 The characterization
of biomatrix using SEM and FTIR spectroscopy indicated
the presence of several functional groups for binding metal ions.
The role of calcium and magnesium present in the biomatrix in the
ion-exchange mechanism has also been reported. The ultimate
maximum adsorption capacity obtained from the Langmuir
isotherm increased in the following order (mmol/g): Ni
(0.094), Zn (0.124), Cd (0.149), Mn (0.151), Co (0.162), Cu
(0.172), Hg (0.18), and Pb (0.28). The adsorption of Cr(III) onto
biomatrix at pH 2 was 1.0 mmol/g. Speciation of chromium,
cadmium, and mercury loaded on the biomatrix was performed
by X-ray photoelectron spectroscopy (XPS).
4.3. Removal of Heavy Metals by Rice Husk Ash. Rice husk
ash (RHA) has been reported to have good adsorptive properties
and is utilized for the adsorptive removal of metal ions from
wastewater. RHA was reported to be a good adsorbent for the
removal of Hg(II) from aqueous solutions and indicated that the
percent adsorption decreased with increased initial concentra-
tion of Hg(II) and the particle size of the adsorbent.75 With an
initial concentration of 100 mg/L of Hg(II), an adsorbent dose of
20 g/L of RHA (diameter of 37
50 μm) removed 98% of the
Hg(II) from their aqueous solution. A contact time of 3 h was
reported to be optimum and the maximum Hg(II) removal was
observed at pH ∼6.0.
Feng et al.76 tested the adsorption capacity of RHA for the
removal of lead from aqueous solution. The Bangham equation
was used to express the mechanism for the adsorption of Pb ions.
A maximum lead removal was observed at pH ∼5.60 and the
maximum amount of adsorption of lead was 12.63 mg/g. They
extended their studies for the removal of Pb(II) and Hg(II) from
aqueous water on RHA.70 Its adsorption capability and adsorp-
tion rate are considerably higher and faster for Pb ions than for
Hg ions. The finer the RHA particles, the higher the pH of the
solution and the lower the concentration of the supporting
electrolyte, potassium nitrate solution, and the greater the
amount of Pb and Hg ions absorbed on RHA. El-Said et al.49
investigated the adsorption potential of Pb(II) from aqueous
solution on RHA. The maximum adsorption was ∼94.75% for
RHA, at a pH of 4.6 ( 0.5, a contact time of 60 min, and an initial
concentration of 30 mg/L. RHA was reported to be more
favorable than rice husk (RH) in the removal of lead(II) from
aqueous solution.49
Gupta and Rastogi77 investigated the adsorption of cadmium
by nonliving algal biomass. The algal biomass exhibited the
highest cadmium(II) uptake capacity at 25 °C, at the initial pH
value of 5.0 in 55 min and at the initial cadmium(II) ion
concentration of 200 mg L
1. Biosorption capacity decreased
from 88.9 to 80.4 mg g
1 with an increase in temperature from
25 to 45 °C at this initial cadmium(II) concentration. Uptake
kinetics follows the pseudo-second-order model and equilibrium
is well described by Langmuir isotherm. Isotherms have been
used to determine thermodynamic parameters of the process,
viz., free energy change, enthalpy change and entropy change.
FTIR analysis of algal biomass revealed the presence of amino,
carboxyl, hydroxyl, and carbonyl groups, which are responsible
for biosorption of metal ions. Acid pretreatments did not sub-
stantially increase metal sorption capacity but alkali like NaOH
pretreatment slightly enhanced the metal removal ability of the
biomass. During repeated sorption/desorption cycles at the end
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Industrial & Engineering Chemistry Research REVIEW

of fifth cycle, Cd(II) sorption decreased by 18%, with 15
20% Table 11. Adsorption Capacities of Dyes on Rice Husk
loss of biomass. Nevertheless, Oedogonium sp. appears to be a
dye adsorption capacity (mg/g) reference
good sorbent for removing metal Cd(II) from aqueous phase.
The equilibrium adsorption characteristics of Cd(II), Ni(II), Malachite Green 28.00 107
and Zn(II) metal ions from aqueous solutions having respective Direct Red-31 25.63 95
metal ion concentrations in the range of 50
500 mmol/dm3 for Direct Orange-26 19.96 95
bagasse fly ash (BFA) and RHA were studied at different Safranine 760 85
temperatures in the range of 293
323 K.78 An increase in
Acid Yellow 36 86.9 102
temperature is observed to induce a positive effect on the
Basic Green 4 511 104
adsorption process. The heat of adsorption (ΔH0) and change
in entropy (ΔS0) for metal adsorption on BFA and RHA are Basic Red 2 838 90
determined to be within the ranges of 26
44 kJ/mol and Basic Blue 9 312 90
127
194 kJ/(mol K), respectively. The isosteric heat of adsorp- Indigo Carmine 65.90 87
tion was quantitatively correlated with the fractional loading of Foron Brill Red 30 85
metal ions onto adsorbents. The investigations also indicated Safranine 838.00 90
that the BFA and RHA possessed heterogeneous surfaces with Sandolan Blue 12 84
sorption sites that had different activities. Solar Blue 38 84
RHA is also reported to be an effective adsorbent for the re- Sandocryl Orange 27 105
moval of Cd(II) and Hg(II) metal ions from aqueous solution.79 Lanasyn Black 9 105
Maximum adsorption for both Hg(II) and Cd(II) metal ions was
Acid Yellow 36 86.9 102
found to occur at pH0 ∼6.0. The affinity of RHA for Cd(II) ions
Congo Red 14.00 149
was observed to be higher than that for Hg(II). The adsorption of
Pb(II) ions from aqueous solution using RHA was investigated, Rhodamine B 5.87  10
5 111
and the adsorption kinetics indicated that the process was Safranine 178.10 110
physisorption-controlled and the pseudo-second-order rate Methylene Blue 280 85
equation suitably interpreted the overall process.80 Methylene Blue 312 90
In another study, the adsorption of Pb(II) ions from aqueous Methylene Blue 40.6 94
solution was investigated on RHA.81 Optimum conditions for Methylene Blue 19.77 107
the removal of Pb(II) ions were reported to be pH 5, an
adsorbent dosage of 5 g/L of solution, and an equilibrium time
of 1 h. The adsorption capacity of RHA for Pb(II) ions was husk (QRH) as an adsorbent for reactive dyes. Lakshmi et al.87
reported to be 91.74 mg/g. The change of entropy (ΔS0) and carried out a study on the adsorptive characteristics of Indigo
enthalpy (ΔH0) were 0.132 kJ/(mol K) and 28.923 kJ/mol, Carmine (IC) dye from aqueous solution onto RHA. Adsorption
respectively. The value of the adsorption energy (E), using the of IC on RHA was favorably influenced by an increase in the
Dubinin
Radushkevich isotherm, was 9.901 kJ/mol and indi- temperature of the operation. The positive values of ΔS0 and the
cated that the adsorption process was chemical in nature. heat of adsorption (ΔH0), and the negative value of the change in
Recently, El-Said82 made an attempt to utilize RHA for the Gibbs free energy (ΔG0,) indicated the feasible and spontaneous
removal of Zn(II) and Se(IV) from their aqueous solution. The adsorption of IC on to RHA. Investigations were made for the
adsorption capability and adsorption rate were reported to be removal of color from aqueous solutions of Methylene Blue (MB)
considerably higher and faster in the case of Zn(II) ions than that and Congo Red (CR) using RHA as an adsorbent.88 The maximum
of Se(IV) ions. They have used the Bangham equation to express percentage removal of MB was 99.94%, while 98.83% removal
the mechanism of adsorption. was reported for CR. Sensitivity analysis further indicated that
the effects of initial dye concentration, shaker speed, pH, and
ionic strength had no noticeable effect on the percentage dye
5. RICE HUSK AS AN ADSORBENT FOR DYE REMOVAL removal at equilibrium. Batch desorption indicated that 50% of
Dyes and pigments are discharged into the water bodies from acetone solution was optimum for CR, while the desorption of
various industrial sources, mainly from the dye manufacturing MB varied directly with acetone concentration.
and textile finishing industries. There are several methods The adsorption of Neutral Red onto RH was reported by Zou
available for the treatment of dye-containing wastewaters. et al.89 The Langmuir adsorption capacities of Neutral Red onto
Among them, the adsorption process provides an attractive RH were 25.16, 29.15, and 32.37 mg/g at 288, 308, and 318 K,
alternative for the treatment of wastewaters, especially if the respectively. The process mechanism was reported to be com-
adsorbent is inexpensive and does not require additional pre- plex, consisting of both surface adsorption and pore diffusion.
treatment before its application. The adsorption capacities of The authors also indicated that the intraparticle diffusion was not
various dyes onto rice husk (RH), modified RH, and rice husk the rate-controlling step and the adsorption process was sponta-
ash (RHA) are shown in Tables 11 and 12. RH is insoluble in neous and endothermic in nature. RH that was obtained from a
water, and it has good chemical stability, high mechanical local rice mill, ground, sieved, washed, and then dried at 80 °C
strength, and a granular structure, making it a good adsorbent was used for the removal of safranine and Methylene Blue, and
material. the respective adsorption capacities were reported to be 838 and
The McKay research group83
85 first investigated the removal 312 mg/g.90 RHA has been used as an adsorbent for the removal
of color, using RH as an adsorbent. Few works have been of Acid Violet 54, Acid Violet 17, Acid Blue 15, Acid Violet 49,
reported on the removal of reactive dyes using RH. However, and Acid Red 119 and their chemical oxygen demand (COD)
Low and Lee86 have reported their studies on quaternized rice from aqueous solutions.91 The adsorption capacity was reported
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Industrial & Engineering Chemistry Research REVIEW

Table 12. Adsorption Capacities of Dyes on Modified Rice Batch experiments were carried out for the adsorption of
Husk and Rice Husk Ash Methylene Blue onto RH particles.94 The monolayer adsorption
capacity of RH for Methylene Blue adsorption was reported to be
adsorption
40.58 mg/g. The adsorption process was controlled by both
dye capacity (mg/g) reference surface and pore diffusion, with surface diffusion at the earlier
oxalic acid-modified Methylene Blue 53.21 107 stages, followed by pore diffusion at the later stages. The authors
rice husk suggested that external mass transfer is the rate-limiting step in
EDTA-RH Methylene Blue 46.30 143
the adsorption process.
RH was also investigated for the removal of Direct Red-31 and
Direct Orange-26 from aqueous solutions.95 Thermodynamic
oxalic acid-modified Malachite Green 54.02 107
studies have indicated that the process was feasible and sponta-
rice husk neous at all temperatures and was endothermic in nature. Surface
NaOH-modified Malachite Green 17.98 106 adsorption of both the dyes at specific binding sites was
rice husk confirmed through FTIR spectroscopic analysis. The authors95
investigated the changes in surface morphology of RH before and
EDTA-RH Reactive Orange-16 7.68 143 after adsorption through SEM analysis and reported that, on the
surface of Direct Red-31 and Direct Orange-26, the formation of
RH Everdirect Orange-3GL 28.41 101 a white monolayer (molecular cloud) covering appeared after the
CMC-RH Everdirect Orange-3GL 23.36 101 adsorption process. The confirmation of monolayer coverage
PVA-alginate Everdirect Orange-3GL 6.89 101
was done by the Langmuir adsorption isotherm. The adsorption
of Brilliant Green (BG) on RHA has been reported by Mane
HCl-RH Everdirect Orange-3GL 30.96 101
et al.96 Intraparticle diffusion does not seem to control the BG
removal process. The adsorption of BG on RHA is favorably
RH Direct Blue-67 50.00 101 influenced by an increase in the temperature of the operation.
CMC-RH Direct Blue-67 28.17 101 The high negative value of ΔG0 indicates the feasible and
PVA-alginate Direct Blue-67 3.83 101 spontaneous adsorption of BG on RHA.
HCl-RH Direct Blue-67 50.0 101 Rice husk modified with oxalic acid (MRH) was tested for the
removal of Neutral Red (NR) dye from aqueous solutions.97 The
rice husk ash Congo Red 171 150 mechanism of the process was complex, consisting of both surface
adsorption and pore diffusion. The values of the effective diffusion
rice husk ash Methylene Blue 690 93 parameter (Deff) were estimated to be of the order of 10
8 cm2/s,
which indicated that intraparticle diffusion was not the rate-control-
ling step. The carboxyl groups on the surface of the modified rice
rice husk ash Indigo Carmine 65.91 87
husk (MRH) were primarily responsible for the adsorption of
NR. The authors97 suggested that MRH may be suitable as an
rice husk ash Brilliant Green 24.20 96 adsorbent material for adsorbing NR from aqueous solutions.
rice husk ash Brilliant Green 26.20 96 Phosphoric acid (H3PO4)- and sodium hydroxide (NaOH)-
treated rice husks, followed by carbonization in a flowing
to vary from 99.4 mg/g to 155 mg/g, making RHA a good nitrogen, were tested for the adsorption of Malachite Green
material. Furthermore, a time period of 30
120 min was (MG) from aqueous solution.98 It is interesting to note that MG
observed to be optimum for attaining equilibrium. adsorbed preferably on carbon-rich sites, rather than on silica-
Experiments have been carried out to characterize the adsorp- rich sites. The behavior of the H3PO4-treated adsorbent followed
tion of MB and CR dyes in the aqueous phase onto RHA.92 The both the Langmuir and Freundlich models, whereas the NaOH-
effective pore diffusivities of the dye molecules investigated in treated adsorbent followed only the Langmuir model. It is
RHA are determined by a suitable global optimization technique. believed that the MG is preferably adsorbed on the carbon
The authors92 have theoretically predicted concentration profiles surface, because the presence of silica, to a certain extent, can
with the experimental values at different initial concentrations of retard the adsorption capacity. RH was also used as the precursor
these dyes, and they indicated that the predicted values are in material by chemical activation with KOH and NaOH at lower
excellent agreement with the experimental values. The possible temperatures.99,100 In another study, free, carboxymethyl cellu-
utilization of an adsorbent for the removal of Brilliant Blue FCF lose (CMC)-immobilized, poly(vinyl alcohol) (PVA)-alginate
dye from aqueous solutions has been investigated.93 Two waste immobilized and chemically treated rice husk was utilized for the
materials—bottom ash, a power plant waste, and de-oiled soya, adsorption of Everdirect Orange-3GL and Direct Blue-67 dyes
an agricultural waste—are meticulously and successfully used as from aqueous solution.101 The maximum adsorption capacity of
adsorbent. For both the systems Langmuir and Freundlich free, immobilized, and hydrochloric acid (HCl)-treated biomass
adsorption isotherm models were applied and, based on these was observed for both dyes at low pH. Comparative investigation
models, useful thermodynamic parameters were calculated. By of free, immobilized, and HCl-treated rice husk showed that the
percolating the dye solution through fixed-bed columns the HCl-treated biomass exhibited greater adsorption capacity for
bulk removal of the Brilliant Blue FCF was carried out and Everdirect Orange-3GL and Direct Blue-67 (29.98 and 37.92
necessary parameters were determined to find out the percen- mg/g, respectively). The Langmuir Type I and Type II models
tage saturation of both the columns. Recovery of Brilliant Blue were best fitted to experimental data for free-, CMC immobi-
FCF was made by eluting dilute NaOH of pH 11 through each lized-, PVA-alginate immobilized-, and HCl-treated rice husk in
column. the case of Everdirect Orange-3GL, while the equilibrium data of
13599 dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research
Direct Blue-67 followed the Langmuir Type II isotherm. Pseudo-
second-order and Elovich kinetic models illustrated good fitness
to all types of rice husks, showing the chemisorption nature of
adsorption, and indicated that adsorption was spontaneous at
high temperature.
Malik102 reported that both Langmuir and Freundlich models
could be used to represent the trends of adsorption on Acid
Yellow 36 dye. His findings indicate that Acid Yellow 36 is
favorably adsorbed by the activated rice husk. However, some
studies have reported that the adsorption data were well-fitted in
the Freundlich isotherm.103
105 However, Guo et al.103,104 em-
phasized that the Freundlich model is not valid for their works.
Moreover, the model is used only to provide a simple representa-
tion of the trends that they observed.
Rice husk treated with NaOH was tested for the removal of MG
from aqueous solution in batch adsorption mode.106 The adsorption
was reported to be strongly dependent on the pH of the medium.
Their studies showed that the mechanism governing the adsorp-
tion process was chemical ion exchange and the rate constant
increased with increasing temperature, indicating the endother-
mic nature of adsorption. Thermodynamic studies suggested the
spontaneous and endothermic nature of adsorption of MG by
treated rice husk. The isosteric heat of adsorption (ΔHX)
increased with increasing surface loading, indicating that chemi-
cally modified rice husk has an energetically heterogeneous
surface and there may be some lateral interactions between the
adsorbed dye molecules. The authors106 concluded that chemi-
cally modified rice husk could be an alternative economic
material to more-costly adsorbents used for dye removal in
wastewater treatment processes.
The adsorption of MB and MG, onto RH and MRH, was
studied in a batch adsorption system.107The mechanism of the
process was complex, consisting of both surface adsorption and
pore diffusion. The thermodynamic investigation showed that
the adsorption of MB and MG onto MRH was feasible, sponta-
neous, and endothermic. The removal capacities of RH and
MRH for the adsorption of dyes from aqueous solution were
compared. By functionalizing, the adsorption capacity (qe) of rice
husk for MB or MG was increased from 19.77 mg/g to 53.21 mg/g
or from 28.00 mg/g to 54.02 mg/g at 293 K, respectively. The
carboxyl groups on the surface of the MRH were primarily
responsible for the adsorption of dyes. Gupta et al.108 investigated
the removal of Safranin-T from wastewater using activated rice
husk. The adsorption of the dye was reported to follow the
Langmuir and Freundlich adsorption isotherm models. The ad-
sorption of Safranin-T over activated rice husks follows first-order
kinetics and the rate constants for the adsorption processes
decreased with increasing temperature.
A factorial experimental design technique was utilized to
investigate the adsorption of Reactive Red RGB from a water
solution on rice husk treated with nitric acid.109 The factorial
design of experiments is investigated to examine the effect of pH,
temperature, adsorbent dosage, and initial concentration of the
dyes, and the most significant variable was reported to be pH of
the solution. Comparison analysis of the linear least-squares
method and the nonlinear method for the estimation of isotherm
parameters on the adsorption of safranin onto RH was made,110
and this analysis indicated that the nonlinear method could be a
better way to obtain the isotherm parameters. Attempts were
made to utilize RH as a potential adsorbent for the removal of a
hazardous xanthene dye, Rhodamine B, from wastewater.111 A
significant decrease in the COD values was reported, which
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clearly indicated that adsorption methods offer good potential to
remove Rhodamine B from industrial effluents.
6. RICE HUSK AS AN ADSORBENT FOR PHENOL, AND
ITS USE IN THE REMOVAL OF OTHER ORGANIC
COMPOUNDS
Phenols and other harmful organic compounds are generally
considered to be among the important organic pollutants
discharged into the environment; these pollutants give water
an unpleasant taste and odor. The major sources of phenol
pollution in the aquatic environment are wastewaters from paint,
pesticide, coal conversion, polymeric resin, and the petroleum
and petrochemicals industries. The adsorption process is effi-
cient for the removal of organic matter from waste effluents.
The adsorption capacity of various phenols and other organic
compounds onto rice husk (RH) and rice husk ash (RHA) are
reported in Table 13.
Because the main components of RH are carbon and silica
(15%
22% SiO2 in a hydrated amorphous form, like silica gel), it
has the potential to be used as an adsorbent for the removal of
phenol and other organic compounds.112,113 Silica is composed
of SiO4 3 4H2O, where each O atom is shared between two
adjacent tetrahedrons. The Si
O bond is ∼50% ionic, because
of the large difference in the electronegativity of oxygen and
silicon. Thus, the ionic structure of silica provides a capability of
adsorbing phenolic compounds, which are polar molecules.114
The adsorption potential of chemically and thermally treated rice
husk (RHT) for the removal of 2,4-dichlorophenol (DCP) from
aqueous solutions has been investigated.115 Maximum adsorp-
tion (98% ( 1.2%) was achieved for RHT from 6.1  10
5
mol dm
3 of adsorbate solution using 0.1 g of RH for 10 min of
agitation time at pH 6 and 303 K, which is comparable to that of
activated carbon commercial (ACC) (96.6% ( 1.2%), but
significantly higher than that of chemically treated rice husk
(RHCT) (65% ( 1.6%) and rice husk untreated (RHUT) (41% (
2.3%). The negative values of enthalpy, entropy, and free energy
suggests that the adsorption is exothermic, stable, and sponta-
neous in nature. The potential of RH and RHA for phenol
adsorption from aqueous solution was studied.116 A comparative
study showed that RHA is more effective than RH for phenol
removal. The adsorption of phenol from aqueous solution is
dependent on the pH of the solution, which affects the surface
charge of the adsorbent, the degree of ionization, and the
speciation of the adsorbate species.116 The amount adsorbed
was reported to decrease with increasing pH value. This may be
attributed to the dependency of phenol ionization on the pH
value. The equilibrium time required for the adsorption of
phenol on rice husk and its ash are almost 6 and 3 h, respectively.
The adsorption process may be considered to be very fast,
because of the large amount of phenol attached to the adsorbent
within the first 120 min of adsorption. RHA would require less
residence time for the complete removal of phenol, compared to
rice husk.116 The studies showed that the RHA can be used as an
efficient adsorbent material for the removal of phenolic materials
from water and wastewaters.
Ahmaruzzaman and Sharma117 investigated the potential of
RH, and rice husk char, for the removal of phenols from waste-
water. The adsorption capacities of RH and rice husk char for
phenol were observed to be 4.50 and 7.90 mg/g, respectively.
They extended their studies for the removal of p-chlorophenol
and p-nitrophenol onto RH and its char. The order of adsorption
dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

Table 13. Adsorption Capacities of Phenols and Other activated carbon, were 0.951, 1, 0.989, and 1 mg phenol/g
Organic Compounds on Rice Husk and Rice Husk Ash adsorbent, respectively.
RH was chemically impregnated with ZnCl2 and carbonized at
adsorption
700 °C in a large-scale rotary furnace and utilized for the removal
capacity (mg/g) reference of humic acid, phenol, and a municipal solid waste landfill
rice husk phenol 4.508 117 leachate.120 The activated rice husk that was obtained had a
rice husk phenol 0.0022 116 Brunauer
Emmett
Teller (BET) surface area of 811 m2/g; this
rice husk p-chlorophenol 14.36 117
material was essentially microporous and showed the best
adsorption behavior toward phenol, removing ∼80% at the
rice husk p-nitrophenol 15.31 117
equilibrium time of 4 h. The adsorption isotherms for humic
acid were also favorable, although the maximum loadings
methacrylic acid- paraquat 317.7 130 achieved were lower than that of phenol. In another study, rice
modified rice husk husk activated carbon obtained using phosphoric acid through
precarbonization and chemical activation has been examined for
rice husk char phenol 7.91 117 the adsorption of phenol from aqueous solutions.121 The surface
rice husk char p-chlorophenol 36.23 117 area, pore volume, and pore size distribution of carbon samples
rice husk char p-nitrophenol 39.21 117 activated at three different temperatures of 700, 800, and 900 °C
have been investigated by these authors. They showed that the
rice husk ash phenol 0.886 116 adsorption decreased with increasing pH and temperature. The
rice husk ash phenol 143.99  10
4 118
adsorption process was exothermic, and the maximum uptake of
phenol was 2.35  10
4 mol/g.
rice husk ash phenol (RHA, 300 °C) 0.951 119
The utilization of RHA as an adsorbent for the adsorption of
rice husk ash phenol (RHA, 400 °C) 1.00 119
humic acids from water was studied.122 The optimum conditions
rice husk ash phenol (RHA, 500 °C) 0.989 119 for the adsorption of humic acid were found in batch method as
rice husk ash resorcinol 888.59  10
5 118 follows: equilibrium time = 60 min and initial pH range = 3
4. In
rice husk ash 2-chlorophenol 209.55  10
6 118 addition, RHA was functionalized with 3-aminopropyltriethoxy-
rice husk ash pyridine 11.72 41 silane and the adsorption behavior of the modified rice husk ash
rice husk ash α-picoline 15.46 30 (RHA-NH2) was investigated.122 The optimum conditions for
rice husk ash humic acid 2.7 122 the adsorption of humic acid were reported to be an equilibrium
time of 30 min and an initial pH in the range of 3
4. The
activated rice phenol 27.58 120 adsorption capacity of RHA-NH2 was higher than that of RHA.
husk ash
The experimental adsorption data fitted well with the Langmuir
equation, and the maximum adsorption capacity was 8.2 mg/g at
pH 6. The comparative adsorption efficiencies of RHA-NH2 and
RHA-NH2 humic acid 8.2 122
commercial activated carbons showed insignificant differences.
The RHA-NH2 adsorbent was also applied for the removal of
activated rice husk ash humic acid 21
45 123 humic acid from surface water. RH was pretreated by HCl,
thermally activated at 700 °C, and chemically modified via an
capacities was reported to be in the following order: phenol < p- aminopropylation reaction with 3-aminopropyltriethoxysilane
chlorophenol < p-nitrophenol.117 and found to be a suitable adsorbent for the adsorption of humic
RHA obtained from a rice mill in Kenya has been used as an acid (HA) from water.122 The adsorption behavior of the
inexpensive and effective adsorbent (and reagent) for the re- prepared adsorbent was best-represented by the Langmuir iso-
moval (and detection) of phenolic compounds in water.118 Their therm. In the column system, the results revealed the feasibility of
studies included the removal of phenol, 1,3-dihydroxybenzene using the adsorbent derived from RHA in water treatment. The
(resorcinol), and 2-chlorophenol from water; and the detection adsorbabilities toward HA of the prepared adsorbent and the
of 1,2-dihydroxybenzene (pyrocatechol) and 1,2,3-trihydroxy- commercial powder activated carbon are not significantly different.
benzene (pyrogallol) present in an aqueous medium. RHA Rice husk was chemically activated with phosphoric acid and
exhibited reasonable adsorption capacity for the phenolic com- utilized for the removal of humic acid from aqueous solution.123
pounds and followed both the Langmuir and Freundlich iso- The monolayer capacity was increased by 38% in the presence of
therm models. For the detection experiments, pyrocatechol Ca2+ and only 4% of the adsorbed HA desorbed. The presence of c-
and pyrogallol that was present in water formed colored com- ations (e.g., Ca2+, Mg2+, Na+, and Al3+) revealed that the humic
plexes with RHA, with the rate of color formation increasing acid uptake was enhanced by certain cationic species and the Ca2+
with temperature, weight of RHA, concentration of the pheno- species showed the greatest effect. A mixed effect of “electrostatic
lic compounds, and sonication.118 The intensity of the color attraction” and “surface complex formation” was suggested to be
formation was reported to increase with contact time, dose of responsible for the adsorption of HA onto the surface of carbon.123
RHA, and concentration of the phenolic compounds. Their Investigations were made to carry out the adsorption capac-
findings indicated that RHA could be utilized as an inexpensive ities of RHA and commercial-grade granular activated car-
“reagent” to detect the presence of phenolic compounds in water. bon (GAC) for the removal of α-picoline (Pi) from aqueous
Investigations were made on the liquid-phase adsorption of solutions.30 The maximum uptake of Pi was observed to be 2.34
phenol from aqueous solutions by RHA and granular activated mg/g at lower concentration (50 mg dm
3) and 15.46 mg/g at
carbon.119 The maximum phenol adsorption capacities of RHA higher concentration (600 mg/dm3), using 20 kg m
3 of RHA,
prepared at 300, 400, and 500 °C, as well as that of granular and the maximum uptake of Pi by GAC was observed to be
13601 dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research
4.55 mg/g at lower concentration (50 mg/dm3) and 36 mg/g at
higher concentration (600 mg/dm3), using 10 kg/m3 of GAC at
normal temperature. Thermodynamic study revealed that the
adsorption of Pi onto RHA and GAC is an endothermic process.
The isosteric heat of adsorption was reported to decrease with
increased surface loading. The acidic water and dilute acids
showed higher desorption efficiency for Pi from RHA and
GAC. They extended their work on the removal of pyridine
from synthetic aqueous solutions using RHA.41 The adsorption
of pyridine is reported to be endothermic in nature, and it can
be recovered from the spent adsorbents, using acidic water and
0.1 N H2SO4.
Silica-incorporated aluminum (RHA-Al) was synthesized
from RHA, using the sol
gel technique.124 RHA-Al was calcined
at 500 °C for 5 h to yield RHA-Al(C). The BET analysis of RHA-
Al(C) showed an increase in total pore volume and specific
surface area, compared to RHA-Al. SEM and XRD showed that
RHA-Al and RHA-Al(C) were composed of microcrystals and
the surface of both samples had a porous structure. Adsorption
studies of palmytic acid on RHA-Al and RHA-Al(C) at 30, 40,
and 50 °C conformed to the Langmuir isotherm.124 The
equilibrium parameter (R) revealed that both are good adsor-
bents for palmytic acid. The Gibbs free energy of adsorption
(ΔG0ads) was determined to be between
21.0 and
26.0 kJ
mol
1, and the values for ΔH0ads and ΔS0ads for RHA-Al were
reported to be 26.2 kJ mol
1 and 158 J mol
1, respectively.
Corresponding values for RHA-Al(C) were 31.7 kJ mol
1 and
178 J mol
1. The adsorption of fatty acid on RHA-Al and RHA-
Al(C) was an endothermic process, which occurred sponta-
neously. An FTIR study on the adsorbed material was utilized
to determine the possible adsorbed complex on the surface of the
adsorbent.
7. RICE HUSK AS AN ADSORBENT FOR SURFACTANT
REMOVAL
Surfactants are synthetic organic chemicals used in high volumes
in detergents, personal care products, and household cleaning
products. These compounds usually comprise 10%
18% of
granular and liquid detergents. Surfactants are also used by the
oil, textile, food, and mining industries. Although there are many
surfactant types, linear alkyl-benzene sulfonates (LABS), alkyl
sulfates (AS), alkyl ether sulfates (AES), alkyl ethoxylates (AE),
alkyl phenol ethoxylates (APE), and quaternary ammonium halide
compounds are common in commercial detergent applications.
Raw domestic wastewaters have LABS concentrations in the
range of 0.54
21 mg/L.125,126 Therefore, the removal of LABS
was needed from the ecotoxicological perspective, because the
toxicity of LABS to aquatic organisms is of concern when the
concentrations exceed 0.1 mg/L. APE materials are nonionic
surfactants that are composed of a branched chain ethylene oxide
to produce an ethoxylated chain. APE are among the most widely
used groups of surfactants. Worldwide, ∼500 000 tons are
produced annually for use in detergents, paints, pesticides, textile
and petroleum recovery chemicals, metalworking fluids, and
personal care products.
A few investigations have been reported on the adsorption of
surfactant by rice husk (RH) from their aqueous solution. The
potential for the utilization of quarternized rice husk (QRH) as
an adsorbent for the removal of linear alkyl benzenesulfonate
from aqueous solution was investigated.127 The removal of linear
alkyl increased as the temperature increased from 4 °C to 50 °C;
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thereafter, uptake remained constant with further increases in
temperature. The presence of anions such as Cl
, H2PO4
,
H2PO4
2, and SO4
2 had little effect on adsorption. Experi-
mental data could be fitted into the Langmuir isotherm with a
maximum sorption capacity of 243.9 mg/g at pH 2.2 and 28 (
2 °C. In the column studies, investigations showed that a linear
relationship existed between service time and bed depth.127
However, the flow rate of influent had no effect on breakthrough
time once it was above 10 mL/min. The ability of RH and its ash
as a low-cost adsorbent for the removal of anionic and nonionic
surfactants in wastewater has been carried out.128 The maximum
removal efficiency of anionic surfactant was reported to be 97%
in aqueous solution, which contains 10 mg/L of sodium linear
alkyl sulfonate in pH 2 and for nonionic surfactants was 75%,
which contains 10 mg/L nonyl phenol ethoxylate in pH 6
7.
The physicochemical characteristics of the RH, the size of
micelles, and the critical micelle concentration (CMC) are the
important properties that affect the adsorption process. The
authors’ findings on the adsorption of surfactants on husk ash
showed that the ash was not responsible for the adsorption
process.128 Because of the long chains of surfactant, there is a
strong van der Waals force between the surfactants and the cellulose
chain, which provides more-desirable conditions for adsorption.
8. RICE HUSK AS AN ADSORBENT FOR PESTICIDES
REMOVAL
The increasing use of pesticides in agriculture, forestry, and
domestic activities for controlling pests is polluting our water
resources day by day. The leaching runoff from agricultural and
forest lands, deposition from aerial applications, and discharge of
industrial wastewater are responsible for this water contamina-
tion. The pesticides form a strong class of water pollutants,
because they are sometimes nonbiodegradable and, moreover,
pesticides are carcinogenic in nature. Therefore, the toxicity of
pesticides and their degradation products makes these chemical
substances a potential hazard by contaminating our environment.
Rice husk (RH) can be utilized for the removal of pesticides
from wastewaters. However, very few studies were reported in
the literature for the removal of pesticides from wastewaters.
Adsorption potential of rice bran and RH for the removal of
triazophosphate (TAP), which is an organophosphate pesticide,
has been reported.129 Rice bran showed higher removal efficiency
(98% ( 1.3%) than RH (94% ( 1.2%). The energy of adsorption
of rice bran and RH was reported as 14 ( 0.1 and 11 ( 0.2
kJ mol
1, respectively, and the kinetics of the adsorption was
reported as 0.016 ( 0.002 and 0.013 ( 0.002 min
1, respec-
tively. Intraparticle diffusion rate was observed to be 4 ( 0.8 and
4 ( 0.9 mol g
1 min
1/2.
Hsu and Pan130 investigated the adsorption of paraquat from
aqueous medium using a methacrylic acid-modified rice husk
(MAA-RH). The carboxyl groups were chemically bound to the
surface of the RH by graft copolymerization using Fenton’s
reagent as a redox initiator. The graft copolymerization was
examined to determine the H2O2 concentration and the amount
of MAA monomer used. FTIR spectra confirmed the presence of
carbonyl groups on the structural units of the rice husk derivative.
The MAA-RH materials were hydrolyzed to sodium salt and used
to adsorb paraquat. The adsorption was rapid in the first few
minutes and quickly reached equilibrium. Equilibrium adsorp-
tion data are more consistent with the Langmuir isotherm
equation than with the Freundlich equation. The maximum
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Industrial & Engineering Chemistry Research
adsorption capacity of modified rice husks was reported as 317.7
mg/g, which is higher than that for Fuller’s earth
(60 mg/g) and activated carbon (90 mg/g).
The potential of RH for the removal of methyl parathion
pesticide (MP) from surface and ground waters has been
reported.131 The maximum capacities of RH for MP were
observed to be 4.7 ( 1.0 mmol/g (using the Freundlich
isotherm), 0.35 ( 0.008 mmol/g (using the Langmuir isotherm),
and 0.9 ( 0.07 mmol/g (using the D-R isotherms). Application
of first-order Lagergren and Morris
Weber equations to the
kinetic data yielded correlation coefficients that were close to unity.
Thermodynamic parameters of the adsorption process (i.e., ΔH,
ΔS, and ΔG) were reported and their negative values indicated
the exothermic and spontaneous nature of sorption process. The
pesticide may be stripped by sonication with methanol, making
the regeneration and reutilization of sorbents promising.
9. RICE HUSK AS AN ADSORBENT FOR INORGANIC
ANIONS REMOVAL FROM WASTEWATER
Apart from the heavy-metal ions in the wastewater, some other
inorganic anions (phosphates, fluorides, boron, etc.) also exist in
waters and could be dangerous to human health. Phosphate
loading to surface water and groundwater from concentrated
agricultural activities (including soil fertilization, feed lots, di-
aries, and pig and poultry farms) is causing water quality problems
in rivers, lakes, etc. Fluoride in drinking water in excess of
desirable levels has been a serious threat to public health. Fluoride
content in groundwater that is greater than the World Health
Organisation (WHO) limit of 1.5 mg/L, causes dental and
skeletal fluorosis. Because fly ash is enriched with the oxides of
aluminum, iron, calcium, and silica, fly ash emerges as a potential
candidate to treat phosphate-laden effluents, since aluminum,
iron, and calcium are known to strongly adsorb or precipitate
phosphates in many agricultural, industrial, and environmental
applications.
The efficiency of fluoride removal from water by rice husk ash
(RHA) was investigated.132 The authors compared the efficiency
of fluoride removal from water with other adsorbents (such as
egg shell and activated carbon); they also examined the potential
of mixed adsorbents for fluoride removal. The investigations
showed that RH had an efficiency of fluoride removal that
exceeded 40%. The egg shell adsorbent had the highest fluoride
removal efficiency, at 61.8%, followed by activated carbon
(53.4%) and RHA (42.5%), and the mixed adsorbents showed
fluoride reductions up to 62%. RH was chemically impregnated,
followed by physical activation, and investigated for the removal
of fluoride from aqueous solution.133 Maximum fluoride removal
was reported to be 75% under optimum conditions. The uptake
of fluoride is possible in the pH range of 2
10, and adsorption
reached a maximum at a lower water pH (pH 2). The authors
suggested that it is preferable to carry out defluoridation at lower
pH values, and fluoride removal increases with time, attaining
equilibrium within 1
1.5 h. Majumder et al.134 investigated the
potential of iron-impregnated active silica
carbon composite
char derived from RH for the treatment of fluoride from
synthetic wastewaters. The authors carried out the process using
wastewater containing 5 ppm fluoride and reported that, after
adsorption, the concentration of fluoride was in the range of
1
2.5 ppm. In another study, RHA was surface-modified by
coating with aluminum hydroxide and utilized for the removal of
fluoride from waters.135 The investigations showed excellent
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fluoride removal efficiency, and the adsorption capacity was
determined to be in the range of 9
10 mg/g.
Phosphate—a compound that has phosphorus as its key
atom—from excess fertilizers and detergents ends up washing
into lakes, creeks, and rivers. This overabundance of phosphorus
causes excessive aquatic plant and algae growth and depletes the
supply of dissolved oxygen in the water. Activated charcoal was
produced from RH, using the steam oxidation process and
utilized for the adsorption of phosphate from wastewater and
compared with activated charcoal from corncob and groundnut
shells and corncobs.136 It was reported that corncob charcoal was
more effective for the adsorption of phosphate than both RH and
groundnut shell and the experimental data obeys the Freundlich
isotherm at all concentrations; the values of adsorption equilib-
rium constants obtained from the adsorption isotherm are 0.9957,
1.000, and 0.9978 for groundnut shell, corncob, and RH charcoals,
respectively. In another study, aluminum-doped rice husk ash-derived
silica (Al-RHA) was synthesized via the cogelation method and
applied as an adsorbent for the removal of phosphate from
wastewaters.137 Al-RHA exhibited fast adsorption kinetics as well
as high adsorption capacities. The optimum phosphate removal
was determined for an initial concentration of 0.3 mg PO4
3/L
with 0.3 g of adsorbent dosage under acidic conditions after 3 h.
The regenerated Al-RHA was reported to have 76% phosphate
removal capacity after being recycled once. The amount of
adsorbent and initial concentration of phosphate solution had little
effect on the concentration of residual Al ions, whereas the con-
centration of residual Al ions decreases with increasing solution pH.
RH was investigated in the denitrification of wastewater in up-
flow laboratory reactors.138 The highest rates of denitrification
(∼0.096 kg/m3 d) were achieved when rate flow and nitrate
concentration were 41.4 L/d and 25.0 mg/L, respectively. Flow
rate and nitrate concentration of the influent were observed to have
a significant effect on nitrate removal efficiency. A very sharp decline
was observed when the flow rate reached a value of 30 L/d. The
reactor had the ability to accommodate a wide range of pH
(6.5
8.5) and dissolved oxygen (DO) (1.5
4). A time-dependent
decrease in nitrate removal rate was observed after 72 days of
operation. They138 indicated that RH could be an economical and
effective carbon source for the removal of nitrate. Orlando et al.139
transformed several natural materials that comprised RH into anion
exchangers and compared their nitrate adsorption capacities. They
observed that lignin was the dominant reactive component respon-
sible for the adsorption of nitrate from their aqueous solution and
cellulose, which is the supporting material for the exchangers.
10. CRITICAL ASSESSMENT OF ADSORPTION
RESEARCH
There has been a large increase in adsorption-related research
for the removal of pollutants from wastewater during the last
several years. However, it is not clear whether such a dramatic rise
in published output has significantly improved any academic
contribution or value to the existing knowledge/understanding
of adsorption from this type of research or aided any commercial
exploitation. Most of the adsorption research involved the
following: (i) selection of an organic material as new adsorbents;
(ii) characterization of a chosen adsorbent materials utilized in
the adsorption of a given substances/pollutants from aqueous
solution; (iii) effect of physicochemical parameters on adsorption;
(iv) carry out simple batch tests and, in some cases, column tests
with new adsorbents; and (v) curve fitting with some well-known
dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research
isotherm and kinetic equations. Theoretically, almost all organic
materials may have some adsorption capacity toward organic com-
pounds or heavy metals, i.e., they may all be used or claimed as
adsorbents. Therefore, there is hardly any novel concept in the
adsorption research and all isotherm and kinetics models used are
well-known and documented in the literature. A major portion of
such studies involved metals, although an increasing number
involved organic pollutants, such as phenols, dyes, and pesticides.
The output of publications shows no sign of abating and will be
increased by the continuing numbers of peer-reviewed journals as
well as new journals, including those that are web-based.
11. MULTICOMPONENT ADSORPTION
Industrial effluents generally contain various types of heavy
metals, along with other organic compounds, such as phenols,
dyes, various salts, and inorganic anions; hence, the design of
adsorption systems should be based on multicomponent sys-
tems. Thus, multicomponent adsorption is very important in
water and wastewater treatment, because most metal ions to be
adsorbed exist in solution with other adsorbable metal ions. The
amount of adsorbed ions depends on the equilibrium between
adsorption competition from all the cations, ionic size, stability of
bonds between the pollutants (metals, dyes, phenols, pesticides,
etc.) and the adsorbent.
Sirvastava et al.140 investigated the competitive adsorption of
cadmium (Cd(II)) and nickel (Ni(II)) ions from aqueous
solution onto rice husk ash (RHA). RHA is reported to be an
effective adsorbent for the removal of Cd(II) and Ni(II) metal
ions from aqueous solution. Higher percentage of metal ion
removal was possible, provided that the initial adsorbate con-
centration in the solution was low. In the binary metal mixtures,
the affinity of the RHA for Ni(II) ions was greater than that for
Cd(II), from both single-component and the binary solutions
under the same experimental conditions. The net interactive
effect of Cd(II) and Ni(II) ions on the adsorption of Cd(II) ions
by RHA was found to be antagonistic. The simultaneous
adsorption phenomena of Cd(II) and Ni(II) ions on the RHA
were explained by various multicomponent equilibrium sorption
models. The adsorption capacities for the binary mixture
RHA
systems are given in the following order: Ni(II) > Cd(II).
They141 also reported the competitive adsorptive removal of
Cd(II) and Zn(II) ions from binary systems using RHA. The
initial pH (pH0) significantly affects the capacity of RHA for
adsorbing the metallic ions in the aqueous solution. The pH0
value of ∼6.0 is determined to be the optimum for the removal of
Cd(II) and Zn(II) ions by RHA. The adsorption of the Zn(II)
ion is reported to be greater than that of the Cd(II) ion, and this
trend is in agreement with the single-component adsorption
data. The equilibrium metal removal decreases with increasing
concentrations of the other metal ions and the combined effect of
Cd(II) and Zn(II) ions on RHA is generally found to be
antagonistic. They142 extended their studies for the competitive
adsorption of Cd(II), Ni(II), and Zn(II) ions onto RHA from
ternary metal-ion mixtures. The equilibrium metal removal
decreases with increasing concentrations of the other metal ions,
and the combined action of Cd(II), Ni(II), and Zn(II) ions on
RHA is found to be antagonistic. The competitive Sheindorf

Rebuhn
Sheintuch (SRS) model fits the ternary adsorption
equilibrium data satisfactorily. The authors142 reported that RHA
is an effective adsorbent for the individual and competitive
removal of Cd(II), Ni(II), and Zn(II) metal ions from aqueous
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solution. In the ternary metal-ion mixtures, the affinity of the
RHA for Zn(II) ions was marginally higher than that for Ni(II) or
Cd(II), for both the single and ternary metal-ion systems. On the
basis of Marquardt’s percent standard deviation (MPSD) error
function, the simultaneous adsorption phenomena of Cd(II),
Ni(II), and Zn(II) ions on the RHA can be satisfactorily and
adequately represented by the SRS model.
EDTA-modified rice husk (ERH) was reported as an adsor-
bent for the removal of both MB and Reactive Orange-16
(RO16) dyes in single and binary systems.143 The optimum
pH for the removal of MB was in the pH range of 4
9, whereas,
for the removal of RO16, an optimum pH value of 2 was
observed. An increasing trend was observed for the removal of
dyes in both single and binary systems when the adsorbent
dosage and agitation rate increased. The removal of MB
decreased with increasing temperature, whereas an opposite
trend was reported for the removal of RO16. The particle size
of the adsorbent seems to have apparent effect on the adsorption
of MB and RO16 in single and binary systems; that is, a decrease
in particle size causes an increase in the percent removal of dye.
A significant increase in the percentage uptake of RO16 was
reported in binary systems, compared to single-component
systems, which indicates that there is a synergistic effect between
the adsorbed dye molecules.143 Gupta et al.144 investigated the
removal of Reactofix golden yellow 3 RFN from aqueous
solution using wheat husk-An agricultural waste. Their findings
showed that the adsorbent has great affinity for the dye. The
effect of various parameters is reported in the paper.
The competitive adsorption of Cd(II) and Hg(II) ions onto
RHA from single-component and binary systems was reported.79
The pH of the system increases during the initial adsorption
process for ∼60 min and remains constant thereafter. The
equilibrium adsorption data were obtained at different initial
concentrations (C0 = 10
100 mg/L) unde rthe following condi-
tions: contact time, 6 h; temperature, 25 °C; RHA dosage, 10 g/L
at pH0 6. The adsorption capacity of Cd(II) is higher than that
for Hg(II) for the binary metal solutions and is in agreement with
the single-component adsorption data. The equilibrium metal
removal decreased with increased concentrations of other metal
ion and the combined action of Hg(II) and Cd(II) ions on RHA
is generally found to be antagonistic. Desorption studies showed
that nitric acid is the best solvent; the maximum elution was
∼28.41% for Cd(II) and ∼31.53% for Hg(II).
12. ADSORPTION ISOTHERM, KINETICS, AND
MECHANISM
The Langmuir and Freundlich isotherms were generally used
to describe observed adsorption phenomena of various metal ions
onto rice husk (RH) and ash. However, other isotherms, such as
Redlich
Peterson, Toth, Dubinin
Radushkevich, Sips, Frumkin,
Harkins
Jura, Halsey, Henderson, and Temkin isotherms, were
also utilized for the same. Most of the reported studies suggested
the applicability of the Langmuir isotherm model (see Table 14).
However, some groups of researchers reported that both the
Langmuir and Freundlich isotherms are applicable to the adsorp-
tion equilibrium data. Bhattachaya et al.59 reported that both the
Langmuir and Freundlich adsorption isotherm models were fitted
well to represent the adsorption of Zn (II) onto rice husk ash
(RHA). These equilibrium isotherm equations are utilized to
describe the observed experimental adsorption data. The different
equation parameters and the underlying thermodynamic
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Industrial & Engineering Chemistry Research REVIEW

Table 14. Applicable Isotherm, Kinetic Models, and Thermodynamic Parameters on the Adsorption of Heavy Metals, Dyes,
Phenols, and Other Organic Compounds

Thermodynamic Parameters

applicable isotherm applicable kinetic
ΔG (kJ/mol) ΔH0 (kJ/mol) ΔS0 (kJ/(K mol)) reference
0

adsorbate models models

RHA Ni(II) Toth 14.82 37.93 162.83 78

RHA Ni(II) Freundlich, Langmuir pseudo-second order 51
RHA Zn(II) Langmuir, Freundlich Lagergren first-order 8.964 59
RHA Zn(II) Toth 17.57 33.35 157.87 78
RHA Pb(II) 13.70 28.92 0.13 81
RHA Pb(II) Langmuir pseudo-second order 49
RHA Pb(II) Langmuir, Freundlich 70
RHA Hg(II) Langmuir, Freundlich 70
RHA Cd(II) 14.19 40.21 166.89 78

RH Pb(II) Langmuir pseudo-second order 49

RH Cr(VI) Freundlich 3.899
4.757
3.032 112
RH Direct Red-31 Langmuir pseudo-second-order 2.949 40.846 143.822 95
RH Direct Orange-26 Langmuir pseudo-second-order 0.2264 64.989 213.625 95
RH Everdirect Langmuir Type-I pseudo-second-order
1.23 13.31 39.28 101
Orange-3GL and Type-II and Elovich

CMC-modified RH Everdirect Langmuir Type I pseudo-second-order
1.67 9.95 27.13 101

Orange-3GL and Type II and Elovich
PVA-alginate-RH Everdirect Langmuir Type I pseudo-second-order
5.80 19.76 54.81 101
Orange-3GL and Type II and Elovich
HCl-RH Everdirect Langmuir Type I pseudo-second-order 0.38 47.30 153.59 101
Orange-3GL and Type II and Elovich

RH Direct Blue-67 Langmuir Type II pseudosecond-order
0.82 40.64 130.1 101

and Elovich
CMC-modified RH Direct Blue-67 Langmuir Type II pseudo-second-order
1.98 11.21 31.07 101
and Elovich
PVA-alginate-RH Direct Blue-67 Langmuir Type II pseudo-second-order
6.09 23.03 54.99 101
and Elovich
HCl-RH Direct Blue-67 Langmuir Type II pseudo-second-order 0.64 22.91 78.05 101
and Elovich

EDTA-RH MB Freundlich pseudo-second order
16.83 30.32 143

oxalic acid- MB Freundlich pseudo-first-order,
12.67 6.42 0.063 107
modified RH pseudo-second-order

EDTA-RH Reactive Freundlcih pseudo-second order 14.95 15.76 143

Orange-16

Acid-RH Cd(II) Langmuir, Freundlich pseudo-second-order 77

Oxalic acid- MG Langmuir pseudo-first-order and
13.04 12.41 0.084 107

modified RH pseudo-second-order
NaOH-treated RH MG Freundlich pseudo-second-
6.18 63.76 234.4 106
order model

methacrylic acid- Paraquat Langmuir
9.6811 130

modified rice husk

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Industrial & Engineering Chemistry Research
Table 14. Continued
applicable isotherm
adsorbate models
rice husk ash α-picoline Radke
Prausnitz
isotherm, Toth,
Redlich
Peterson
RH phenol Freundlich first-order
RHA phenol Freundlich first-order
RHA Brilliant Green Redlich
Peterson, pseudo-second-order
dyes Langmuir
assumptions of these models often provide insight into both the
adsorption mechanism, and the surface properties and affinity of
the adsorbent. Therefore, it is important to establish the most
appropriate correlation of equilibrium curves to optimize the
condition for designing the adsorption systems. Various re-
searchers have used these isotherms to examine the importance
of different factors on various pollutants adsorption by RH and
ash. Linear regression was frequently used to determine the most
frequently used model throughout the years.
Several kinetic models, such as Lagergren’s first-order model,
the pseudo-second-order model, and the Elovich model, have
been reported in the literature to describe the kinetics of the
adsorption process. The Lagergren’s first-order equation and the
pseudo second-order equation are the most widely used kinetic
models to describe the adsorption of a solute from a liquid
solution (Table 14). The pseudo-second-order kinetic models
were reported to explain the adsorption process in most of the
cases.49,51,95,107,143 The pseudo-second-order rate expression was
used to describe chemisorption involving valence forces through
the sharing or exchange of electrons between the adsorbent and
adsorbate as covalent forces, and ion exchange.
The major challenge in an adsorption study is to elucidate the
mechanism of adsorption. However, before understanding the
adsorption mechanism, one must also consider the structure of
the adsorbate and the surface properties of the adsorbent. To
understand the mechanism of the adsorption, various processes,
such as FTIR spectroscopy, attenuated total reflection
infrared
(ATR-IR) spectroscopy, X-ray diffraction (XRD), electrophore-
tic mobility (EM), extended X-ray absorption fine structure
(EXAFS) spectroscopy, as well as SEM and TEM, are used.
The mechanisms reported in the literature included hydrogen
bonding, chemical adsorption, ion exchange, and precipitation.
For most cases, chemisorption is reported to be the main
mechanism of metal ions at high pH values. The surface
complexation model is usually applied to simulate the adsorption
data of metal ions on different solid particles. In many other
cases, surface complexation and ionic exchange were considered
as the main mechanisms under different experimental conditions.
Zou et al.107 investigated the removal of MB and MG onto natural
and oxalic acid-modified rice husk and suggested that the main
mechanism for the adsorption behavior of MB and MG onto MRH
was ion exchange. They also reported that the removal process was
complex, consisting of both surface adsorption and pore diffusion.
However, the mechanism for the removal of MG by adsorption on
REVIEW
Thermodynamic Parameters
applicable kinetic
ΔG (kJ/mol) ΔH0 (kJ/mol) ΔS0 (kJ/(K mol)) reference
0
models

15.110 20.965 0.127 41
116
116

46.51 28.30 0.23 96
treated rice husk is reported to involve the formation of surface
hydrogen bonds between the hydroxyl groups on the RH surface
and the N atoms of MG or through a dye-hydrogen ion exchange
process.106 Safa and Bhatti95 suggested that the adsorption of direct
dyes onto RH is not dependent only on intraparticle diffusion: other
mechanisms might be involved. Their findings also indicated that
chemisorption mechanisms are involved in the adsorption of Direct
Red-31 and Direct Orange-26 dyes on RH.
13. EFFECTS OF VARIOUS PARAMETERS ON THE AD-
SORPTION PROCESS
Many factors can affect the adsorption process. The type,
nature, and source of the biomass or derived waste products can
be very important, including the nature of its applications. Physical
and chemical treatments will also affect binding properties, while
chemical treatments such as alkali treatment often improve the
adsorption capacity. Apart from these, other physicochemical
factors, such as pH, the presence of other anions and cations, initial
concentration, particle size of adsorbents, pollutant solubility and
form, and temperature, also influence the adsorption process.
13.1. Effect of Initial Concentration and Contact Time. The
initial concentrations of adsorbate have a strong effect on the
adsorption capacity of rice husk (RH) and its ash. Adsorption
capacity is generally increased with increased initial concentra-
tion of the adsorbates. The initial concentration provides an
important driving force to overcome all mass-transfer resistance
of adsorbate between the aqueous and solid phases. Choudhury
et al.106 investigated the effect of initial dye concentration on the
adsorption of MG, using treated rice husk. The initial dye
concentration increased from 10 mg/L to 100 mg/L, the adsorp-
tion capacity of the treated rice husk increased. It is reported that
adsorption of α-picoline increased with an increase in initial
concentration of α-picoline (Pi) and attributed to the increase in
the mass-transfer driving force, because of an increase in initial
concentration.30 The capacity of HA adsorption also increases
with rising initial concentration of the solute, up to 35 and
50 mg/L for rice husk ash (RHA) and RHA-NH2, respectively.
Above this concentration, the equilibrium was reached probably
because of the limited number of active sites available to adsorb
HA on the sorbent surfaces. As anticipated, the large HA mole-
cule could be adsorbed essentially on the external surface or in
wider pores. Thus, upon covering the surface, a second layer was
not favorable.122
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Industrial & Engineering Chemistry Research
The effect of DCP concentration on its adsorption onto RH was
studied over a concentration range of (0.61
6.1)  10
4
mol dm
3, using optimized conditions.115 It was found that the
distribution coefficient (Rd) decreases with the increase in DCP
concentration, up to 4  10
4 mol dm
3 with a gradual fall resulting
in slope, and becomes almost constant from (4
6)  10
4
mol dm
3 of DCP solution. This may be interpreted in terms of
limiting sorption sites, which may not be sufficient to accommodate
an increasing number of 2,4-dichlorophenol molecules available on
the sorbent surface. An increase in the initial concentration of the
metal ions enhanced the adsorption uptake of Cd(II) and Hg(II)
and ions onto RHA.79 The adsorption capacity of Hg(II) is reported
to increase with increase in initial concentration of Hg(II).75 A
similar trend is observed for the adsorption of Zn(II) on RH.64
It is important to evaluate the effect of contact time required to
reach equilibrium for designing batch adsorption experiments.
The effect of contact time on adsorption of MG was investigated,
the adsorption of MG by treated rice husk was reported to be a
function of contact time at different initial concentrations.106 The
adsorption of MG increased with contact time up to 20 min and
further increases in contact time did not enhance the adsorption.
Initially, the rate of adsorption was rapid, because of the adsorp-
tion of dye molecules onto the exterior surface and, after that, the
molecules enter into pores (interior surface), which is a relatively
slow process. The initial faster rates of adsorption may also be
attributed to the presence of a large number of binding sites for
adsorption and the slower adsorption rates at the end is due to the
saturation of the binding sites and the attainment of equilibrium.
The effect of contact time on the removal of α-picoline (Pi) on
RHA initially shows a rapid adsorption of Pi (>75%) up to 15
min; thereafter, the removal of Pi is very sluggish and the initial
sorption rate is rapid, because of the availability of more adsorp-
tion sites.41 Imyim122 investigated the effect of contact time on
the removal of HA onto RHA and RHA-NH2 and the contact
times required to reach adsorption equilibrium were 60 and
30 min for RHA and RHA-NH2, respectively. The adsorption of
MB and MG onto oxalic acid-modified rice husk increased with
increasing contact time at different initial dye concentrations.107
A similar observation is reported for the removal of Methylene
Blue on RHA.27 The effect of contact time on basic dye and acid
dye removal was investigated, and the contact time required to
reach equilibrium for the basic dye is short using RH.105 Mbui
et al.118 studied the effect of contact time on the removal of
phenol and resorcinol and reported that the percentage adsorp-
tion was increased with time and found to be 72%, 52%, and 48%,
for phenol, 2-chlorophenol, and resorcinol, respectively, after
60 min. Their findings also showed that RHA has a higher affinity
for phenol than resorcinol.
13.2. Effect of pH. The pH of the aqueous solution is one of
the most important factors affecting the adsorption process. It
influences not only the surface charge of the adsorbent, the
degree of ionization of the material present in the solution, and
the dissociation of functional groups on the active sites of the
adsorbent, but also the solution solute chemistry. Choudhury
et al.106 studied the effect of pH on the removal efficiency of MG
and reported that the adsorption of MG was strongly pH-
dependent. The equilibrium uptake of dye increased notably as
the pH increased from 2.0 to 4.0; above that, the adsorption
capacity did not change significantly, up to pH 9.0. At low pH
values, the protonation of the functional groups present on the
adsorbent surface easily takes place, and thereby restrict the
approach of positively charged dye cations on the surface of the
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adsorbent resulting in low adsorption of dye in acidic solution. With
decreasing acidity of the solution, the functional groups on the
adsorbent surface become deprotonated, resulting in an increase in
the negative charge density on the adsorbent surface and facilitate
the binding of dye cations. The increase in dye removal capacity at
higher pH also may be explained by the reduction of H+ ions, which
compete with dye cations at lower pH for appropriate sites on the
adsorbent surface. However, with increasing pH, this competition
weakens and dye cations replace H+ ions bound to the adsorbent
surface, resulting in increased uptake of dye.
The effect of the initial solution pH on the amount of MB and
MG ions adsorbed under equilibrium conditions was reported.107
The values of adsorption capacity for RH and MRH were the
smallest at the initial pH of pH0 = 2.0. The lower uptake
capacities of dyes at low pH are probably due to the presence
of excess H+ ions holding the sorption sites on RH or MRH. For
MB or MG basic dye, it will be positively charged in solution. As
the pH of the dye solution becomes higher, the association of dye
cations on the solid will occur more easily, resulting in an increase
in adsorption. For RH, its main functional group is the hydroxyl
group. Along with an increase of the pH value, the concentration
of H+ ions that compete with the dye cations for sorption sites
decreased. The uptake of dyes adsorbed on RH gradually
increased as the initial pH was increased. For MRH, its practical
functional group is the carboxyl group. When the pH was low, the
presence of excess H+ ions could restrain the ionization of the
carboxyl group, so the nonionic form of the carboxyl group
(
COOH) was present. The adsorption capacity of the dyes was
small, because of the absence of electrostatic interaction. When
the pH was high, the carboxyl group is changed to
COO
, and the
adsorption capacity of the dye increased. The values of adsorption
capacity increased as the initial pH increased from pH 1 to pH 7;
insignificant changes were observed beyond pH 7. The uptake of
MB and MG by MRH was much higher, compared to RH.
The adsorption capacity of HA on rice husk ash (RHA)
increased as the initial pH decreased from pH0 5 to pH0 3.122
The maximum adsorption of HA on RHA was reported at pH
3
4, while the constant adsorption capacity was over pH 5. In
the higher pH range (pH > pHZPC, where pHZPC is the pH value
of the zeta potential charge), the silanol groups contribute a
negative charge, and HAs contributes negative charges because of
the dissociation of carboxylic groups.123 Consequently, the uptake
of HA would be reduced. For RHA-NH2, the capacity of HA
adsorption was much higher than that of unmodified RHA. Similar
to RHA, the maximum adsorption was found at pH 3
4. At this
pH range, which is below pHZPC, the amine groups present on the
surface of RHA-NH2 takes up H+ ions from solution and, hence,
the presence of primary ammonium ions or Si
R
NH3+. On the
other hand, HA are predominantly negatively charged due to an
abundance of dissociated carboxylic groups or HA
O
, and it has
been noted that HA
O
will tend to be associated with an
equivalent number of Si
R
NH3+ on the RHA surface.
The effect of pH on the uptake of dodecylbenzenesulfonate
(DBS) by NR and QRH was investigated and reported that QRH
exhibited much higher capability to adsorb DBS than RH in the
pH range of 2
10.127 Feng et al.70 reported that the adsorption
capacity of lead and mercury was low at lower pH and increased
as the initial pH increased, with a more pronounced effect being
observed on lead. The maximum adsorption capacity was
reported with an initial pH of 5.60
5.80. The adsorption of
phenol from aqueous solution is also reported to be dependent
on the pH of the solution.119
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Industrial & Engineering Chemistry Research
The uptake of Zn(II), as a function of hydrogen ion concen-
tration, was examined over a pH range of 3
11, and maximum
removal was obtained in the pH range of 5
7.59 For RHA with
an initial concentration of 25 mg/L of Zn(II), the maximum
removal (96.8%) was obtained at pH 5. The effect of pH can be
explained by considering the surface charge on the adsorbent
material. At low pH, because of the high positive charge density
due to protons on the surface sites, electrostatic repulsion will be
high during the uptake of metal ions, resulting in lower removal
efficiency. With increasing pH, electrostatic repulsion decreases,
because of the reduction of positive charge density on the sorption
sites, thus resulting in an enhancement of metal adsorption.
A similar observation was reported in the adsorption of Cr(IV),
Cu(II), and Cd(II) by RH.57 Tiwari et al.75 also reported that the
adsorption of Hg(II) on RHA was dependent on the solution
pH. The maximum adsorption of Cr(VI) was found in the pH
range below 5, and the adsorbed amount was negligible in pH
values over 8.75 These findings are supported by the work
reported by Sumathi et al.48
13.3. Effect of Temperature. The temperature of the system
plays an important role in adsorption capacity. Thermodynamic
parameters such as standard free-energy change (ΔG0), enthalpy
change (ΔH0), and entropy change (ΔS0) were determined
using the following equation:
ΔG0 ΔS0 ΔH 0
ln Kc ¼
¼
ð1Þ
RT R RT
where Kc is the equilibrium constant that is resulted from the
ratio of the equilibrium concentrations of the adsorbate on the
adsorbent and in the solution, respectively. The linear property
of ln Kc against 1/T has been proven in many studies that have
been reported in the literature. The values of ΔG0 or ΔS0 and
ΔH0 were determined from a plot of ln Kc versus 1/T. A negative
ΔG0 value indicates the process to be feasible and suggests the
spontaneous nature of adsorption. A positive ΔH0 value indicates
the endothermic nature of adsorption, and ΔS0 can be used to
describe the randomness at the solid
solution interface during
the adsorption. In most of the cases, it has been found that the
adsorption capacity increases as the temperature increases.
Table 14 showed the reported values of ΔG0 or ΔS0 and ΔH0
for the removal of metals, dyes, phenols, and other organic
compounds from aqueous solution onto RH and its ash.
Choudhury et al.106 reported that temperature remarkably
influenced the equilibrium dye uptake. The adsorption of dye
increased as the temperature increased, indicating that a high
temperature favored MG removal by adsorption onto chemically
modified rice husk. The enhancement in adsorption, with the
increase in temperature, may be attributed to the increase in
the number of active surface sites available for adsorption, the
increase in the porosity of the adsorbent, and increases in the
pore volume of the adsorbent. An increase in temperature
increases the rate of diffusion of the adsorbate molecules across
the external boundary layer and within the internal pores of the
adsorbent particle, because of a decrease in the viscosity of the
solution. The enhancement in adsorption also may be a result of an
increase in the mobility of the dye molecules with an increase in their
kinetic energy.
The removal of Pi onto RHA was also found to increase with
increasing temperature.41 The increase in adsorption capacity is
probably because of the creation of some new active sites on the
surface of adsorbents. The increase in the adsorption capacity of
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the adsorbents with an increasing temperature indicates that the
adsorption is an endothermic process.41 Lee et al.127 showed that
an increase in temperature from 4 °C to 50 °C increased the
percentage uptake of dodecylbenzenesulfonate onto RH; how-
ever, further increases in temperature did not show any increase
in uptake. The adsorption of phenolic compounds on RHA was
investigated and reported no significant effect on the percent
adsorption of the phenolic compounds.118
14. COLUMN STUDIES
Column-type continuous flow operations possess distinct advan-
tages over batch-type process. The adsorbents are continuously in
contact with a fresh solution in the column operation, and,
therefore, the concentration of the solution in contact with a
given layer of adsorbent in a column is relatively constant. For
batch treatment, the concentration of solute in contact with a
specific quantity of adsorbent steadily decreases as adsorption
proceeds, hence decreasing the effectiveness of the adsorbent for
the removal of solute from their aqueous solution. The column
operation is also important from the practical point of view for
the treatment of real wastewater.
Sumathi et al.48 utilized rice husk (RH) for their effectiveness
in removing chromium from tannery effluent through column
experiments. The adsorption capacity of RH was compared to
that of sawdust, coir pith, and vermiculite. The sawdust exhibited
a higher adsorption capacity, followed by coir pith. About 94%
removal of chromium was achieved by a column of coir pith, and
equally (93%) by a column containing a mixture of coir pith and
vermiculite. Amin et al.54 investigated the possibility of the
utilization of RH without any pretreatment in the removal of
arsenic from aqueous media. Adsorption column methods
showed the complete removal of both As(III) and As(V) under
the following conditions: initial As concentration, 100 μg/L; RH
amount, 6 g; average particle size, 780 and 510 μm; treatment
flow rate, 6.7 and 1.7 mL/min; and pH, 6.5 and 6.0, respectively.
The desorption efficiencies with 1 M of KOH after the treatment
of groundwater were in the range of 71%
96%, and the method
is effective for a wide range of concentrations (i.e., 50
500 μg/L).
The adsorption potential of rice-husk-based activated carbon
(RHAC) to remove Cu(II) from aqueous solution was investi-
gated using a fixed-bed adsorption column.145 The highest bed
capacity of 34.56 mg/g was obtained using a 10 mg/L inlet Cu(II)
concentration, 80 mm bed height, and 10 mL/min flow rate.
Column experiments indicated that the adsorbed amount of
Hg(II) decreased with increasing flow rate and decreasing bed
height.75 Studies using glass columns filled with RH were carried
out at room temperature, employing 100 mL of synthetic solu-
tions containing Cd(II) and Pb(II) at 100 mg/L in order to see
the effects of pH, flow rate, and particle size on Cd(II) and Pb(II)
adsorption.146
The potential of tartaric acid-modified rice husk (TARH) for
the removal of copper and lead from semiconductor electroplat-
ing wastewater was also reported.147 Application of the Langmuir
isotherm indicated that there was no difference in the adsorption
capacity of TARH for copper and lead in synthetic solution and
wastewater. Increases in column bed depth yielded longer service
time, while increases in influent concentration and flow rate
resulted in faster breakthrough. Theoretical breakthrough curves
at different bed heights and flow rates generated using a two-
parameter model agreed closely with experimental values in the
treatment of semiconductor wastewater. The metals, copper and
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Industrial & Engineering Chemistry Research
lead, could be recovered almost quantitatively by eluting the
column with 0.1 M HCl and the column could be used repeatedly
for at least five cycles.
The ability of RH to adsorb Methylene Blue (MB) from
aqueous solution was tested in a fixed-bed column.148 The effects
of important parameters, such as the value of initial pH, ionic
strength the flow rate, the influent concentration of MB, and bed
depth, were studied. When the flow rate was 8.2 mL/min and the
influent concentration of MB was 50 mg/L, the equilibrium
adsorption reached 4.41 mg/g, according to the Thomas model.
They extended their study for the removal of Congo Red (CR)
from aqueous solution, using a continuous bed of RH.149 The
effects of important factors, such as the value of pH, ionic
strength the flow rate, the influent concentration of CR, and
bed depth, were investigated.
RHA obtained by acid washing and calcination at 600 °C was
mixed with kaolin and starch to make pellet adsorbents and
utilized for the removal of CR in a packed column.150 Both ash
and pellet samples showed good adsorption capacities toward the
organic substances in wastewater. Furthermore, the surface
nature of the white ash and pellet adsorbent could be modified
through either hydration or esterification reactions. Correspond-
ing changes in silanol concentrations were successfully correlated
to the changes in adsorption capacity toward CR.
15. DESORPTION STUDIES
The disposal or regeneration of spent adsorbent is one of the
important factors in assessing the feasibility of an adsorption
system151
162 therefore, it is suggested that, as the purchase costs
of the rice husk (RH) is negligible and it is primarily carbona-
ceous and cellulosic, the preferred disposal method is by dewa-
tering, drying, and burning. It was also suggested that the heat of
combustion may be recovered as waste heat and utilized for
drying of the adsorbent and steam generation.
Desorption of the rice-husk-loaded adsorbate (metals, dyes,
phenols, organic compounds, and other inorganic ions) enables
reutilization of RH, as well as the recovery of adsorbed materials.
In some cases, desorption treatments may improve further
adsorption capacities, although in other cases, there may be a
loss of efficiency of the RH. For the operation of continuous flow
systems, columns in parallel arrangements may allow adsorption
and desorption processes to occur without significant interrup-
tion. A variety of substances have been used as metal/radio-
nuclide desorbents, including acids, alkalis, and complexing
agents, depending on the substance adsorbed, the process
requirements, and economic considerations. In addition, there
may be a means of selective desorption (e.g., for certain metals).
Dye-loaded rice husk can be eluted and regenerated by some
organic solvents, such as methanol, ethanol, surfactants, and
NaOH. Distilled deionized water, CaCl2, and NaOH have been
used to desorb phenolic compounds and pesticides.
16. CONCLUSIONS AND FUTURE RECOMMENDATIONS
This review article summarizes the investigations carried out
by various workers on the adsorption of various pollutants from
wastewater onto rice husk (RH) and rice husk ash (RHA). The
optimization of adsorption parameters utilizing RH and its ash
could be achieved by correlating operating parameters and
adsorbent characteristics. It was demonstrated from the literature
that RH has been used as a potential low-cost adsorbent material
for the removal of various pollutants from wastewater. Because of
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the presence of silica, RH exhibited high performance in the
adsorption of various pollutants from wastewater. It was found
that adsorption capacity of RH increased after chemical and
thermal treatment. However, this increase in adsorption capacity
depends on the method and conditions of treatment and also
varies from researcher to researcher. Modification of RH using
some heavy metals can also make them applicable for the
adsorption of inorganic anions via surface precipitation. The
findings will provide a 2-fold advantage, namely (i) a large
volume of RH could be partly reduced, converted to useful,
value-added adsorbents, and (ii) developed low-cost adsorbent
may overcome the wastewaters pollution at a reasonable cost.
Detailed mechanism of contaminant/modification reagent/RH
interactions is required for a better design of adsorption experi-
ments with modified rice husk. In addition, regeneration of spent
RH and disposal of contaminants-loaded rice husk using simple
methods/techniques should also be a focus in future research.
There exists some relationship between adsorption properties
and the structure of the adsorbate or the surface properties and
groups of the adsorbent, besides the porosity/surface area
properties. Although much research has been done on the
adsorption process, there are still many amphibolous matters
for further research, such as the quantificational relationship
between pore size distribution of the adsorbent, size of adsorbate
molecules, functional groups present on the surface of adsorbent,
batch or column conditions, particle size of adsorbent, and the
adsorption capacity, which will help in predicting and selecting
adsorbents in the application of real wastewater treatment. Some
researchers confirmed that the batch technique contains various
sources of uncertainty and brings relevant uncertainty to deter-
mine adsorption parameters. It has been found that experimental
procedure represents important source of uncertainties, and a
great portion of the final distribution coefficient uncertainty
comes from this source. For performance assessment studies in
the future, understanding the variation in distribution coefficient
uncertainty sources is important to weigh the influence of
experimental setup on final adsorption data.
Besides the studies of single-component adsorption of metals,
dyes, phenols, and other organic compounds, multicomponent
adsorption should be addressed in future research. In the literature,
most studies utilizing RH were based on batch mode, highlighting
their applicability and selectivity. However, once conditions of batch
experiment, adsorptive capacity, and mechanism are established,
research work should be conducted to design and carry out pilot-
plant studies to verify their viability at an industrial scale. Moreover,
real wastewater should be tested, instead of synthetically prepared
wastewater. In the wastewater treatment, the interaction among the
different adsobates in solution will play an important role in the
adsorption efficiency of different adsorbates. The adsorbents with
high adsorption capacity, easy separation from aqueous solution,
low cost, and recycling use are promising materials in the future. The
high selectivity for the interested adsorbate is most important for the
materials in the removal of mostly interested adsorbates from large
volumes of aqueous solutions.
’ AUTHOR INFORMATION
Corresponding Author
*E-mail: md_a2002@rediffmail.com.
’ ABBREVIATIONS
RH = rice husk
dx.doi.org/10.1021/ie201477c |Ind. Eng. Chem. Res. 2011, 50, 13589–13613
Industrial & Engineering Chemistry Research REVIEW

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