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Green Technologies for Wastewater Treatment

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 Second International Conference
in New Research on
chemistry & chemical engineering

Green Technologies for Wastewater Treatment

Seyyedeh Cobra Azimi* - Alireza Pendashteh

Environmental Research Institute, Academic Center for Education, Culture & Research (ACECR),
4144635699, Rasht, Iran

ABSTRACT

Chemistry and Chemical technology has contributed considerably to the development of abundant
human life by providing various kinds of useful materials. Although there have been several adverse
effects, the positive effects were dominate. As for the future, we are confident that chemical technology
will continue to play key roles, but we can not foresee similar development as in the past, because of the
limited supply of resources and the intolerable environmental disruption. The influences of science and
technology might have grown beyond our controllability.
The implementation of clean, eco-friendly, less energy and waste producing processes and
technologies is realized today with an increasing interest. In order to provide a sustainable development,
environmentally friendly substances, novel technologies and new green chemistry options should be
utilized. In that respect, in this paper green chemistry, green engineering and their principles are reviewed
in relation to green technologies for wastewater treatment.

Keywords: Green chemistry, Sustainable development, Wastewater treatment.

1. INTRODUCTION

Chemistry has provided valuable materials in the form of medicines, food products, cosmetics,
dyes, paints, agrochemicals, biomolecules, high-tech substances like polymers, liquid crystals and
nanoparticles. Chemists have used their knowledge and skill to prepare a large number of new materials
which are far better and more useful than the natural products, such as high-tech polymers, liquid
crystals, tough ceramics, nonlinear optical substances, novel electronics, designer drugs, genetic materials
and new energy sources. The processes on industrial scale involve many chemical reactions using huge
quantities and wider varieties of smaller molecules, reagents, solvents, acids, alkali, etc. These chemical
processes not only produce the required products but also large quantities of undesired and harmful
substances in the form of solids, liquids and gases and have become the biggest challenge that chemistry
has to face. So, the pressing need for the synthetic chemists is to minimize chemical pollution [1].
Also there is a growing need for more environmentally acceptable processes in the chemical
industry. This trend towards what has become known as green chemistry, clean chemistry, environmental
chemistry, benign chemistry or sustainable technology necessitates a paradigm shift from traditional
concepts of process efficiency, that focus largely on chemical yield, to one that assigns economic value to
eliminating waste at source and avoiding the use of toxic and/or hazardous substances [2-9]. Green
chemistry has become, and still is, the most popular among a number of alternatives.

1.1. Green Chemistry

The term ‘Green Chemistry’ was coined by Anastas [4] of the US Environmental Protection
Agency (EPA). In 1993 the EPA officially adopted the name ‘US Green Chemistry Program’ which has
served as a focal point for activities within the United States, such as the Presidential Green Chemistry

Green Technologies for Wastewater Treatment 1

Challenge. Awards and the annual Green Chemistry and Engineering Conference. This does not mean
that research on green chemistry did not exist before the early 1990s, merely that it did not have the name.
Since the early 1990s both Italy and the United Kingdom have launched major initiatives in green
chemistry and, more recently, the Green and Sustainable Chemistry Network was initiated in Japan. The
inaugural edition of the journal Green Chemistry, sponsored by the Royal Society of Chemistry, appeared
in 1999.
Green Chemistry is defined as the ‘‘design of chemical products and processes to reduce or
eliminate the use and generation of hazardous substances’’ [2,10,11]. The most important aspect of Green
Chemistry is the concept of design. Design is a statement of human intention and one cannot do design by
accident. It includes novelty, planning and systematic conception. The Twelve Principles of Green
Chemistry are ‘‘design rules’’ to help chemists achieve the intentional goal of sustainability. Green
Chemistry is characterized by careful planning of chemical synthesis and molecular design to reduce
adverse consequences.
The Twelve Principles of Green Chemistry are design criteria or guidelines that provide the
framework for sustainable design. They constitute an overarching construct for the design of safer
chemicals and chemical transformations. Chemistry has long been perceived as a dangerous science and
often the public associates the word ‘‘chemical’’ with ‘‘toxic.’’ There are ways to reduce risk by using
safety precautions such as protective gear. When safety protections fail, the risk, which is defined as a
function of the hazard and exposure, increases (Fig. 1). If the hazard is high and exposure controls fail,
the consequences can be catastrophic (injury or death). By minimizing the hazard portion of the equation
instead of focusing only on exposure controls, the risk can be limited even in cases of undesirable
circumstances (accident, spills, sabotage, etc. . .). Designing safer sustainable chemicals and processes
requires striving to reduce the intrinsic hazards to a minimum and therefore limiting the risk of accident
and damage [2,10].
Risk= f (hazard ˟ exposure)
Fig. 1. Risk is a function of hazard and exposure.

The drive towards clean technology in the chemical industry with an increasing emphasis on the
reduction of waste at source will require a level of innovation and new technology that the chemical
industry has not seen in many years. Mature chemical processes, which are often based on technology
developed in the first half of the 20th century, may no longer be acceptable in these environmentally
conscious days. ‘Enviro-economics’ will become the driving force for new products and processes. This
can be seen by considering the ever-escalating and various ‘costs of waste’ (Fig. 2) [12].

Pollution Clean-up costs

Attitutdes of
Energy Inefficiencies Emissions Health and safety issues workforce

Raw materials Attitutdes of neighbours

Environment
inefficiencies

Production Public Relations

COST OF WASTE
Byproduct
generation Tougher legislation
Waste Disposal
Future

Increased costs of disposal Increased cost of technology

Increased cost of raw materials to stav in business
through depletion

Loss of business
Fig. 2. The costs of waste [12].
 Second International Conference
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The main objective of green chemistry is thus, the reduction of this "Costs of Waste". It can be
considered as a series of reductions (Fig. 3). These reductions lead to the goal of triple bottom-line
benefits of economic, environmental, and social improvements. Costs are saved by reducing waste (which
is becoming increasingly expensive to dispose of, especially when hazardous) and energy use (likely to
represent a larger proportion of process costs in the future) as well as making processes more efficient by
reducing materials consumption. These reductions also lead to environmental benefit in terms of both
feedstock consumption and end-of-life disposal. Furthermore, an increasing use of renewable resources
will render the manufacturing industry more sustainable [13]. Careful design will reduce or eliminate
intrinsic hazards within chemicals and processes; a design based on the integration of the twelve
principles as one cohesive set.

Fig. 3. Reducing: The heart of Green Chemistry

1.2. The Twelve Principles of Green Chemistry

The Twelve Principles of Green Chemistry were introduced in 1998 by Paul Anastas and John
Warner (Table 1). They are a guiding framework for the design of new chemical products and processes,
applying to all aspects of the process life-cycle from the raw materials used to the efficiency and safety of
the transformation, the toxicity and biodegradability of products and reagents used.

Table 1. The Twelve Principles of Green Chemistry [14].

Prevention of Waste. It is better to prevent waste than to treat or clean up waste after it is formed.
Atom Economy. Synthetic methods should be designed to maximize the incorporation of all materials
used into the final product as expressed by ‘‘atom economy’’.
Less Hazardous Chemical Syntheses. Wherever practicable, synthetic methodologies should be designed
to use and generate substances that possess little or no toxicity to human health and the environment.
Designing Safer Chemicals. Chemical products should be designed to preserve efficacy of function while
reducing toxicity.
Safer Solvents and Auxilliaries. The use of auxiliary substances (e.g. solvents, separation agents) should
be made unnecessary wherever possible and, innocuous when used.
Design for Energy efficiency. Energy requirements should be recognized for their environmental and
economic impacts and should be minimized. Synthetic methods should be conducted at ambient
temperature and pressure.
Use of Renewable Feedstocks. A raw material of feedstock should be renewable rather than depleting

Green Technologies for Wastewater Treatment 3

wherever technically and economically practicable.
Reduces Derivatives. Unnecessary derivatization (blocking group, protection/deprotection, temporary
modification of physical/chemical processes) should be avoided whenever possible.
Catalysis. Catalytic reagents (as selective as possible) are superior to stoichiometric reagents.
Design products for degradation. Chemical products should be designed so that at the end of their
function they do not persist in the environment and break down into innocuous degradation products.
Analytical methodologies for pollution prevention. Analytical methodologies need to be developed to
allow for real-time, in-process monitoring and control prior to the formation of hazardous substances.
Inherently safer processes. Substances and the form of a substance used in a chemical process should be
chosen so as to minimize the potential for chemical accidents, including releases, explosions and fires.

Failure to follow the simplest rule of green chemistry that is waste prevention has resulted in most
of the troublesome hazardous waste sites that are causing problems throughout the world today. This was
recognized in United States with the passage of the 1990 Pollution Prevention Act. This principle
explicitly states that, wherever possible, wastes are not to be generated and their quantities are to be
minimized. The means for accomplishing this objective can range from very simple measures, such as
careful inventory control and reduction of solvent losses due to evaporation, to much more sophisticated
and drastic approaches, such as complete redesign of manufacturing processes with waste minimization
as a top priority. One of the most effective ways to prevent generation of wastes is to ensure, as much as
possible, the incorporation of all raw materials into the final product. In that respect, the concept of atom
economy defined as Principle 2 is a key component of green chemistry [15]. The remaining principles are
focused on issues such as toxicity, solvent and other media using consumption of energy, application of
raw materials from renewable sources and degradation of chemical products to simple, nontoxic
substances that are friendly for the environment.
Today, the practice of green chemistry enables designing chemicals and new approaches in a way
that effectiveness is retained and even enhanced while toxicity is reduced. Chemical syntheses as well as
many manufacturing operations make use of auxiliary substances that are not part of the final product.
The use or generation of substances that pose hazards to humans and the environment should be
minimized or totally avoided where the connection between green chemistry and environmental
chemistry is especially strong. Utilization of environmentally acceptable additives for water treatment is
one important area where green chemistry can potentially find applications [16].
While there has been significant focus on designing chemicals for various functions ranging from
medicines to materials, there has been a surprising lack of interest in taking into consideration hazard in
the design process. Understanding the properties of a molecule that have an impact on the environment
and the transformations that take place in the biosphere is essential to sustainability. Through a mastery of
this understanding, chemistry will be able to genuinely design molecules that are safer for humans and the
environment. Work by Ariens [17] in 1984 and by Garrett and Devito in 1996 showed that designing
safer chemicals is not only highly needed for the advancement of Green Chemistry, but is also possible
[18].
Synthesis of an organic compound often results in the generation of byproducts that may require
disposal. Products that must be dispersed into the environment should be designed to break down rapidly
into innocuous products. An example is the synthesis of biodegradable polymers [19]. Another example
would be the modification of the poorly biodegradable surfactant used in household detergents. Their
widespread consumption caused severe problems of foaming in wastewater treatment plants and
contamination of water supplies. Hence, 15 or 20 years after their introduction, they were chemically
modified to yield a product that was a biodegradable substitute.
Solvents are perhaps the most active area of Green Chemistry research [20,21]. They represent an
important challenge for Green Chemistry because they often account for the vast majority of mass wasted
in syntheses and processes [22,23]. Moreover, many conventional solvents are toxic, flammable, and/or
corrosive. Their volatility and solubility have contributed to air, water and land pollution, have increased
the risk of workers’ exposure, and have led to serious accidents. Recovery and reuse, when possible, is
often associated with energy-intensive distillation and sometimes cross contamination. In an effort to
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address all those shortcomings, chemists started a search for safer solutions. Solventless systems [24,25],
water [26,27], supercritical fluids [28,29] (SCF) and more recently ionic liquids [30-32] are some
examples of those new ‘‘green’’ answers. The use of supercritical CO2 as an environmentally friendly
reaction medium for chemical synthesis, product separation and catalyst recycling has recently been
revealed as an interesting clean alternative to classical organic solvents. Among various approaches,
combinations of ionic liquids with supercritical fluids, particularly supercritical CO2, offer a highly
attractive choice.
Energy consumption poses economic and environmental costs in almost all synthesis and
manufacturing processes. In a broader sense, energy requirements should be minimized to avoid potential
threats to the environment. One way to accomplish this goal could be the use of processes that occur at
ambient conditions, rather than options requiring elevated temperature or pressure. A successful approach
has been the application of biological processes for water and wastewater treatment, which, because of
the conditions under which organisms grow, must occur at moderate temperatures and in the absence of
toxic substances.
Raw materials extracted from earth are from a finite supply that cannot be replenished once they
are used. So, wherever possible, renewable raw materials should be used. It has been estimated that the
vast majority of our manufacturing products are derived from petroleum feedstock or natural gas.
[1,10,33]. The depletion of those resources will touch many aspects of our consumer life and our
economy. Turning towards renewable feedstocks both for material and fuel has now become more urgent.
The major renewable feedstock on the planet both for material and energy is bio-mass [33], the material
available from living organisms. This includes wood, crops, agricultural residues, food, etc [34].
Examples of renewable material include cellulose, lignin, suberin and other wood compounds, poly
hydroxyl alkanoates, lactic acid, chitin, starch, glycerol and oil. Chitin is an abundant natural polymer that
constitutes the exoskeleton of arthropods (e.g. crustaceans). It is a major byproduct of the seafood
industry and can be transformed into chitosan by deacetylation [35]. Numerous applications of chitosan
have been described from water purification, biomedical applications and other industrial uses [36,37].
Covalent derivatization is a ubiquitous technique in chemistry whether it is employed for organic
synthesis or analytical chemistry [38]. In many cases, the formation of waste is linked to the traditional
use of a stoichiometric amount of reagents [39]. Switching from stoichiometric methodologies to catalytic
processes is perceived as one major way to improve the efficiency of the synthetic toolbox. Catalysis can
improve the efficiency of a reaction by lowering the energy input required, by avoiding the use of
stoichiometric amount of reagents, and by greater product selectivity. This implies less energy, less
feedstock and less waste [40].
Attaining ‘‘real-time’’ control of chemical processes by modern computerized systems is
important for efficient and safe operation with minimum production of wastes. However, accurate
knowledge on the concentrations of materials used in the system is required. Therefore, the successful
practice of green chemistry requires real-time, in-process monitoring techniques coupled with process
control. Accidents, such as spills, explosions, and fires, are a major hazard in the chemical industry. They
are not only potentially dangerous, but also tend to spread toxic substances into the environment and
increase exposure of humans and other organisms to these substances. For this reason, it is best to avoid
the use or generation of substances that are likely to react violently, burn, build up excessive pressures, or
otherwise cause unforeseen incidents in the manufacturing process [40].
During the last two decades, with the establishment of sustainable development as a goal for
society, several concepts for environmental management, that look for strategies different than just
complying with environmental regulations have evolved. Aiming to achieve sustainability by introducing
environmental considerations in human activities, the specific response of the chemical industry in this
context has become to apply the concept of green chemistry. A definition of the most common and
accepted concepts of green chemistry for environmental management as presented by Munoz are
introduced in Table 2 [41].

Green Technologies for Wastewater Treatment 5

 Table 2. Concepts related to green chemistry [41].
Green engineering. Green engineering is the design, commercialization and use of economically feasible
processes and products while minimizing pollution and any threat to human and the environment.
Cleaner Production. Continuous use of an integrated and preventive environmental strategy to processes,
products and services to increase the eco-efficiency and reduce risks to population and the environment.
Eco-efficiency. It is achieved by the delivery of competitively priced goods and services that satisfy
human needs and bring quality to life while reducing ecological impacts throughout life cycle in line with
Earth’s estimated carrying capacity.
Industrial Ecology. Examination of industry and environment where industrial system is visualized as a
producer of both products and wastes and understanding the relationship between producers, consumers,
other entities and the natural world.
Ecodesign. Designing products and minimizing their direct or indirect impacts at every possible
opportunity.
Life cycle Thinking. A way of addressing environmental issues and opportunities from a systematic
perspective. It involves evaluating a product or service with the goal of reducing potential environmental
impacts over the entire life cycle.

1.3. The Twelve Principles of Green Engineering

Unfortunately, the twelve principles of green chemistry do not explicitly include a number of
important concepts, highly relevant to environmental impact; for example, the inherency of a product or
process, the need for life cycle assessment, or the possibility of heat recovery from an exothermic reaction
or heat integration. For this reason, Anastas and Zimmerman [42] subsequently proposed a set of 12
principles of green engineering (Table 3). The 12 Principles of green engineering (Table 3) provide a
framework for scientists and engineers for designing effective, ecologically intelligent materials,
products, and systems [43]. This approach builds on the technical excellence, scientific accuracy, and
systematic thinking that have addressed in recent years the issue of science and technology for
sustainability and sustainable development.

Table 3. The Twelve Principles of Green Engineering [42].

Principle 1. Designers need to strive to ensure that all material and energy inputs and outputs are as
inherently non hazardous as possible.
Principle 2. It is better to prevent waste than to treat or clean up waste after it is formed.
Principle 3. Separation and purification operations should be a component of the design framework.
Principle 4. System components should be designed to maximize mass, energy and temporal efficiency.
Principle 5. System components should be output pulled rather than input pushed through the use of
energy and materials.
Principle 6. Embedded entropy and complexity must be viewed as an investment when making design
choices on recycle, reuse or beneficial disposition.
Principle 7. Targeted durability, not immortality, should be a design goal.
Principle 8. Design for unnecessary capacity or capability should be considered a design flaw which
includes engineering ‘‘one size fits all’’ solutions.
Principle 9. Multi component products should strive for material unification to promote disassembly and
value retention (minimize material diversity).
Principle 10. Design of processes and systems must include integration of interconnectivity with
available energy and materials flows.
Principle 11. Performance metrics include designing for performance in commercial ‘‘after life’’.
Principle 12. Design should be based on renewable and readily available inputs throughout the life cycle.
Incorporating green engineering design principles within engineering education with specific
examples for chemical engineering was revealed by Shonnard et al. [44]. The application and efficacy of
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green chemistry and other green design principles were documented for many case studies, including
biodegradable polymers, and the production of polymers from biomaterials [45].
Green engineering, along with green chemistry, are engaged through science and technology on
ensuring that quality of life, or state of economic development is increasing through benign chemicals,
materials and life cycle-based design [2]. A relationship linking environment, green engineering, green
chemistry and sustainability are shown in Fig. 4.

Fig. 4. Relationships among environment, sustainability, green engineering and green chemistry.

The need to use resources efficiently and reduce environmental impacts of industrial products and
processes is becoming increasingly important in engineering design; therefore, green engineering
principles are gaining prominence.

2. Results and Discussions

2.1. Green Technology
The objectives of water and wastewater treatment green technologies are: (i) to reduce and
conserve the use of water and associated non-renewable energy sources; (ii) to prevent contamination and
misuse of water and other natural resources; (iii) to protect biodiversity, habitats, and ecosystems, and (iv)
to ensure that future generations can meet their own needs. Taking into account current public concern on
environmental matters, the consequent use of toxic reagents and solvents have increased to a point at
which they became unsustainable to continue without an environmentally friendly perspective. The
concept of embodying the chemical water treatment in green chemistry was presented by Ghernaout et al.
[46] with a specific example addressing the unavoidable role of chlorination. Detailed investigation was
devoted to the question of how the chemical water treatment with its chlorination in the forms of pre-
disinfection, disinfection, and post-disinfection and coagulation using alum could be turned in a green
water treatment.
Another emerging field for water and wastewater treatment is the application of advanced
oxidation oxidation processes (AOPs). These processes are based on the production of highly reactive
radicals, especially hydroxyl radicals, which promote destruction of the target pollutant until
mineralization. These radicals can be produced by means of oxidizing agents such as O 3, H2O2, ultraviolet
irradiation, ultrasound, and catalysts (homogeneous or heterogeneous).

2.1.1. Advanced Oxidation Processes

Advanced oxidation processes (AOPs) are defined as a set of chemical treatment processes
designed to remove organic compounds in wastewater by several oxidation reactions. In order to generate
highly reactive intermediates, OH radicals, the AOPs may proceed along one of the two routes given
below [47]:

Green Technologies for Wastewater Treatment 7

  Use of high energy oxidants such as ozone and H2O2 and/ or photons. The generation of
hydroxyl radical might possibly be by the use of UV, UV/O3, UV/H2O2, Fe+2/H2O2, TiO2/
H2O2 and a number of other processes [48].
 Use of O2 in temperature ranges between ambient conditions and those found in
incinerators, such as in wet air oxidation (WAO) processes in the region of 1-20 MPa and
200-300 °C.
The technologies that can be classified as AOPs fall under two general categories in terms of
whether UV source is used in the process. Table 4 shows the classification of AOPs [49]. In recent years,
the research found in literature has shown that toxic and refractory organics in wastewater could be
destroyed by most AOPs, such as ozonation, photocatalytic degradation, Fenton’s reagent (H 2O2/Fe2+),
photo-Fenton, and wet air oxidation, and have proven to be very effective for dye-containing effluents
[50-52]. Various combinations of these AOPs may also provide efficient removal of dyes from aqueous
media.

Table 4. Classification of Advanced Oxidation Processes [49].

Non-photochemical Photochemical
Ozonation Photocatalytic oxidation, UV/Catalyst
Ozonation with hydrogen peroxide (O3/H2O2) UV/H2O2
Fenton (Fe2+ or Fe3+ /H2O2) UV/O3
Wet air oxidation (WAO) UV/O3/H2O2
Electrochemical oxidation Photo-Fenton (Fe3+/H2O2/UV)

2.1.1.1. Nonphotochemical Advanced Oxidation Processes

There are several well known methods for generating hydroxyl radicals without using light energy.
These are ozonation, Fenton’s reagent oxidation, wet air oxidation and electrochemical oxidation.

2.1.1.1.1. Ozonation
Ozone and ozone-based advanced oxidation processes are powerful, environmentally friendly
technologies capable of degrading a variety of organic pollutants [53]. Ozonation is the method which is
widely preferred for removal of colored substances since the chromophore groups with conjugated double
bonds, which are responsible for color, can be easily broken down by ozone, either directly or indirectly
forming smaller molecules [54]. The ozonation process is realized in three steps:
 Generation of ozone
 Dissolution of ozone in the wastewater
 Oxidation of organic matter
In the case where ozone cannot completely oxidize organic compounds to CO2 and H2O due to the
formation of partial oxidation products relatively unreactive towards ozone, the combination of ozone
with homogeneous or heterogeneous catalysts, with or without metallic phases, is recommended for the
enhancement of degradation of organic compounds [55].Up till now, numerous studies have demonstrated
that dyes can be effectively degraded by ozone and some published studies are summarized in Table 5.

Table 5. Summary of some results in the removal of dyes by ozonation [56].

Dye Time Catalyst Color COD TOC
(min) Removal (%) Removal Removal
(%) (%)
Textile Dyeing Factory 360 - 90 - -
wastewater
C. I. Reactive Blue 5 - LaCoO3 - - 100
Acid Red B 60 Fe-Cu oxide 90 70 -
Reactive Blue 19 90 - - 55 17
Procion red MX-5B 30 Metal ions 97 - 75
RR198 9 MgO nanocrystal 100 - -
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catalysts
C. I. Acid Blue 113, C. Less than 10 activated carbon, 100 - -
I. Reactive Yellow 3, C. cerium oxide,
I. Reactive Blue 5 ceria-activated
carbon composite
Reactive Blue 19 10 - BOD/COD=0.33 - -
Bomaplex Red CR-L 10-30 - 100 35-56 -
dye
Acid, Direct and 180 - 100 66 -
Reactive
C. I. Direct Black 22 160 - 70-83 - 33
Red X-GLR 120 - 100 5.7-35 -
Remazol Black 5 360 - - 40 25

2.1.1.1.2. Fenton’s Reagent Oxidation

Fenton’s reagent oxidation is a catalytic oxidation process using a mixture of strong chemical
oxidizer, hydrogen peroxide, and ferrous ions as a catalyst and an acid as an optimum pH adjuster. This
particular reagent mixture is called Fenton’s Reagent. The main advantages of Fenton’s reagent oxidation
compared to other AOPs are its simplicity, the lack of toxicity of the reagents and the cost effective
source of hydroxyl radicals it offers, since the chemicals are always available at moderate cost and there
is no need for special equipment [57].
The general mechanism using Fenton’s reagents, via which the hydroxyl radicals are produced, is
a number of cyclic reactions, which utilize the Fe2+ or Fe3+ ions as a catalyst to decompose the H2O2 [58].
The efficiency of the treatment can be considerably increased when ultraviolet light is simultaneously
irradiated in the Fenton process, the so called photo-Fenton’s process [59,60]. Under irradiation, ferric ion
complexes produce extra OH radicals and the regeneration of Fe (II), which will further react with more
H2O2 molecules in Fenton reaction. Some studies performed on Fenton’s Reagent oxidation of dye
pollutants are illustrated in Table 6.

Table 6. Summary of some results in the removal of dyes by Fenton’s Oxidation [56].
Dye Time T [H2O2] Catalyst pH Color COD TOC
(min) (°C) (mM) Removal Removal Removal
(%) (%) (%)
Reactive - 30 4.0 iron (III) 3 89.18 - -
Black 5 impregnated on
rice husk ash
Alcian - 50 30.0 - 2.5 93.2 - 54.1
Blue
Reactive - 30 4.0 iron (III) 3 89.18 - -
Black 5 impregnated on
AC
Reactive 5 - 8.3 - 3 80 - -
Blue 19
C. I. Acid 6 80 8.7 Fe (II)-Y Zeolite 5.9 99 - -
Red 14 6
Reactive 150 - 12 Montmorillonite 2.5 99 - -
Black 5 K10
Acid Red 1 120 30 8.0 iron ions loading 2.0 96 - -
on rice husk

Green Technologies for Wastewater Treatment 9

Direct Blue 50 30 2.8 - 4.0 100 - -
15
Reactive 30 50 - - 3.0 91.4 52.27 -
Yellow
145
Reactive 15 - - - 3.0 97.5 21.6 -
Black 5

2.1.1.1.3. Wet Air Oxidation

The wet air oxidation (WAO) process, which was first patented by Zimmerman over 50 years ago,
removes organic compounds in the liquid phase by oxidizing them using an oxidant such as oxygen or air
at high temperatures (120-300°C) and pressures (0.5-20 MPa) [61,62]. With the help of WAO processes,
the organic contaminants dissolved in water are in turn partially degraded by means of an oxidizing agent
into biodegradable intermediates or mineralized into innocuous inorganic compounds such as carbon
dioxide, water and inorganic salts, which remain in the aqueous phase [63]. The wet air oxidation
mechanism is divided into two steps:
 A physical step, which involves the transfer of oxygen from the gas phase to the liquid
phase, usually considers that oxygen diffuses rapidly within the gas phase, and the
transfer of carbon dioxide to the gas from the liquid.
 A chemical step, which involves the reaction between the organic matter and dissolved
oxygen in the liquid phase, producing carbon dioxide.
Studies on the WAO of some model dyes are listed in Table 7.

Table 7. Summary of some results in removal of dyes by Catalytic Wet Air Oxidation [56].
Dye Time P T Catalyst pH Color COD TOC
(min) (MPa) (°C) Removal Removal Removal
(%) (%) (%)
Reactive 90 - 70 Commercial 3 92 - -
Black 5 activated
carbons
(AquaSorb 5000
P)
Methyl 120 - - CuO/c-Al2O3 - 99 - 70
Orange Direct
Brown Direct
Green
Basic Yellow - - 150 Ni/MgAlO - - - -
11
Acid Orange 7 160 0.5 150 NaNO2/FeCl3 2.6 - - 56
Reactive Dye 120 1.0 135 CoAlPO4-5 - 95 90 -
Solution 165 CeO2 100 95
Orange II 100 0.6- 260 H4SiW12O40, - - - 90
3.0 Na2HPW12O40
Orange II 150 1.0 230 catalyst - - - 70
comprising ZnO,
CuO, and A12O3

2.1.1.1.4. Electrochemical Oxidation

Electrochemical oxidation is another method that belongs to the advanced oxidation methods. The
electrochemical oxidation method is considered an environmentally friendly technology that is able to
electrogenerate in situ hydroxyl radicals [64]. One of the main advantages of the method is that on the
surface of electrodes only electrons are produced and consumed. Electrochemical methods oxidize and
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reduce pollutants in wastewater by means of electrode reactions. The electrodes needed are available in
various shapes (bar, plate, porous and fiber) and are made of various materials; processes are influenced
significantly by the anode material. The requirements for an ideal anode material include acceptable
efficiency, cost-effectiveness and stability in severe conditions [65].

2.1.1.2. Photochemical Advanced Oxidation Processes

To produce photochemical changes in a molecule, irradiation of light in the UV-visible range must
occur within the system. The visible spectrum covers wavelengths between 400 and 800 nm. The most
common sources of UV light are high-pressure mercury vapor lamps and pulsed-UV (P-UV) xenon arc
lamps with good emission [66]. Photochemistry offers numerous advantages over conventional treatment
methods such as lower reaction temperatures and control of selectivity. State of the art of photochemical
processes were addressed and future trends were explained in detail. Implementation of UV irradiation in
sample-preparation and sample introduction systems provides remarkable improvements in analytical
characteristics as well as green methods for trace-element analysis and speciation [67].

2.1.1.2.1. Photocatalytic Oxidation

Direct photolysis involves the interaction of light with molecules to bring about their dissociation
into fragments. Photocatalytic oxidation is a very efficient and promising advanced oxidation process in
which various types of organic compounds can be broken down to CO2, water and mineral salts, and
complete mineralization can be achieved by the help of activated oxygen species such as the hydroxyl
radical and super oxide radicals [68]. The use of semiconductors such as TiO2, ZnO, Fe2O3, and CdS as
photocatalysts is inevitable for the degradation of organic pollution. Due to its optical and electrical
properties, low cost, remarkable photocatalytic activity, chemical stability, nontoxicity and
photocorrosion resistance, nano-titanium dioxide is preferred as a common photocatalyst [69,70]. The
catalytic activity of TiO2 catalyst has been raised by using transition metals. Recently, photocatalytic
degradation of organic pollutants has been improved by immobilization of the transition metals onto solid
matrices such as activated carbon, zeolite, clay, sand, glass, stainless steel and various biomaterials. These
supporting materials provide a large surface area for adsorption, prevent leaching and allow the catalyst
recovery [68,70].
The total degradation of organic pollutants such as dyes, pesticides, surfactants, phenolic
compounds, aromatic, and aliphatic compounds, haloaromatics, nitrohaloaromatics, and amides that can
be photodegraded using TiO2 as catalyst were revealed by Blake [71]. Herrmann et al. [72] the
photocatalytic oxidation of 4-tert-butyl-benzaldehyde was presented as an example of ‘‘green chemistry’’
based on the reasons that air is used and titania catalyst is a cheap, stable, and recyclable material. Some
of these studies are summarized in Table 8.

Table 8. Summary of some results in the removal of dyes by Photocatalytic Oxidation [56].
Dye Time T UV Catalyst Type pH Color COD TOC
(min) (°C) Intensity Removal Removal Removal
mW/cm2 (%) (%) (%)
Reactive Blue - - 32 Watt Nano-titania 3 95.22 - 92.52
2
Acid Yellow - - 25 TiO2 and - - - -
mW/cm2 activated
carbon
Azo dye - - - Iron or - - - -
containing Cesium doped
wastewater nanotitaina
films

Green Technologies for Wastewater Treatment 11

Acid Red 27 - room - Nano ZnO 7 - 100 -
Alizarin 90 - - TiO2- - - - -
Cyanine Activated
Green carbon-TiO2
Methylene 120 - - H4SiW12O40, 6.8 - - -
blue (MB) Na2HPW12O40
Real textile
wastewater
(TW)
Basic Red 18 - - - catalyst - - - -
(BR18) Basic comprising
Red 46 ZnO, CuO,
(BR46) and A12O3

2.1.1.2.2. Ultraviolet Irradiation and Hydrogen Peroxide (UV/H 2O2)

Currently gaining more attention is the UV/H2O2 system, which is an advanced oxidation process
in which hydrogen peroxide (H2O2) is added in the presence of ultraviolet (UV) light to generate hydroxyl
radicals (OH). As reported, hydrogen peroxide is a strong oxidant for reducing low levels of pollutants
present in wastewaters [73]. However, the individual use of H2O2 is not always efficient in oxidizing
more complex pollutants. The use of H2O2 becomes more effective when it acts in conjunction with other
reagents or energy sources capable of dissociating it to generate hydroxyl radicals. Studies on the removal
of dyes using UV/H2O2 have shown that it is a promising method to treat dilute aqueous solutions of azo
dyes [74].

2.1.1.2.3. Photocatalytic Ozonation (UV/O3)

Ozonation combined with ultraviolet (UV) radiation is deemed as a more effective process to
remove organics; compared to sole ozonation, a larger quantity of OH radicals can be formed. UV
radiation is commonly employed to enhance ozone decomposition, yielding more free radicals and
resulting in a higher ozonation rate [75]. The main difference between combined photocatalytic ozone
decomposition and ozone decomposition alone in aqueous solution is the initiation of the reaction. The
starting radical is formed photochemically by an electron transfer from photocatalyst to oxygen and not
by the reaction of OH− ion with ozone [76].

2.1.2. Membrane Bio Reactor (MBR) Technology

The number of MBR technology applications for municipal wastewater treatment has grown
enormously during the last decade. These systems have several environmental advantages with respect to
conventional activated sludge process (high effluent quality, reduced footprint, reduced sludge production
etc.); recently, it has been demonstrated that they improve at higher extent effluent estrogenicity
abatement, even though this positive effect may not be predicted based on trace pollutant concentrations,
being for many substances similar to those obtained by conventional process. On the other hand, higher
environmental costs, mainly due to membrane fabrication/installation and energy consumption for plant
operation, have to be carefully evaluated in order to assess if MBR can be considered to be a green
technology. Membrane Bio Reactor (MBR) is the acronym for water and wastewater treatment processes
which integrates a biological process with a membrane separation step. In general, membrane filtration is
aimed at retaining biomass and other suspended materials so as to produce a clarified and disinfected
permeate. Factors for which MBR may be considered a green technology are directly related to reduced
environmental impact achievable by means of this technology. We can mention in particular the high
effluent quality (as already pointed out), the avoided use of chemicals for disinfection (thanks to the
capability of membranes to retain pathogens), the reduced excess sludge production (which is a
consequence of the generally long SRT), etc. However, as far as trace pollutant removal is concerned,
data reported in the previous paragraph do not seem to show significant and general better performances
of MBR, in comparison with conventional activated sludge process [77].
 Second International Conference
in New Research on
chemistry & chemical engineering

3. Conclution
Achieving the goals of green chemistry and green engineering involves the combined roles to be played at
all aspects of society, government, and industry. Innovation and application of new cleaner technologies
will probably lead to the success realization of the benefits to society and future generations. Increasing
knowledge on the production of oxidative species with higher yields, reaction pathways, reactor design,
process combination, as well as applications for water reuse make AOPs a promising green treatment
technology.

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