Phosphorus Pollution Control Using Waste-Based Adsorbents: Material Synthesis, Modification, and Sustainability

Critical Reviews in Environmental Science and
Technology
ISSN: (Print) (Online) Journal homepage: https://www.tandfonline.com/loi/best20
Phosphorus pollution control using waste-based

adsorbents: Material synthesis, modification, and
sustainability
Hongxu Zhou, Andrew J. Margenot, Yunkai Li, Buchun Si, Tengfei Wang,
Yanyan Zhang, Shiyang Li & Rabin Bhattarai
To cite this article: Hongxu Zhou, Andrew J. Margenot, Yunkai Li, Buchun Si, Tengfei Wang,
Yanyan Zhang, Shiyang Li & Rabin Bhattarai (2022) Phosphorus pollution control using waste-
based adsorbents: Material synthesis, modification, and sustainability, Critical Reviews in
Environmental Science and Technology, 52:12, 2023-2059, DOI: 10.1080/10643389.2020.1866414
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CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY
2022, VOL. 52, NO. 12, 2023–2059
https://doi.org/10.1080/10643389.2020.1866414
Phosphorus pollution control using waste-based

adsorbents: Material synthesis, modification, and
sustainability
Hongxu Zhoua , Andrew J. Margenotb, Yunkai Lic, Buchun Sic,
Tengfei Wangd, Yanyan Zhange, Shiyang Lif, and Rabin Bhattaraia
a
Department of Agricultural and Biological Engineering, University of Illinois at Urbana-
Champaign, Urbana, Illinois, USA; bDepartment of Crop Sciences, University of Illinois Urbana-
Champaign, Urbana, Illinois, USA; cCollege of Water Resources and Civil Engineering, China
Agricultural University, Beijing, P. R. China; dFaculty of Geosciences and Environmental
Engineering, Southwest Jiaotong University, Chengdu, P. R. China; eDepartment of Natural
Resource Sciences, McGill University, Quebec, Canada; fKey Laboratory of Organic Compound
Pollution Control Engineering (MOE), Shanghai University, Shanghai, P. R. China
ABSTRACT
The utilization of waste materials
to control phosphorus (P) pollu-
tion has been intensively studied
as a promising strategy to
achieve sustainable wastewater
treatment. Although many meth-
ods are proposed and investi-
gated to develop modified waste-
based adsorbents, a core yet still-
debated issue is their effective-
ness and viability in real-world applications. Therefore, this critical review summarizes
the current research state on the use of waste materials and their modified forms as
adsorbents for dissolved reactive P removal from wastewater. Various performance
improvement methods are compiled into the research outcomes to highlight three sig-
nificant efforts that scientists have contributed to promoting the application of waste-
based adsorbents: (i) how to enhance the P removal efficiency; (ii) how to scale up
implementation; and (iii) how to achieve sustainable management. Furthermore, this
review proposes a paradigm of waste-based absorbent in the P removal process to sys-
tematically formulate a complete sustainable management strategy for practical appli-
cation. Overall, this review offers a guide for the development and application of
waste-based adsorbents for P removal from wastewater.
KEYWORDS Development and application; phosphorus removal; sustainable management; waste-based

adsorbents; wastewater treatment
CONTACT Shiyang Li lishiyang1987@gmail.com Key Laboratory of Organic Compound Pollution Control

Engineering (MOE), Shanghai University, Shanghai, 200444 P. R. China; Rabin Bhattarai rbhatta2@illinois.edu
Department of Agricultural and Biological Engineering, University of Illinois at Urbana-Champaign, 1304 W.
Pennsylvania Avenue, Urbana, IL 61801, USA.
ß 2021 Taylor & Francis Group, LLC
2024 H. ZHOU ET AL.
1. Introduction
In the past decades, with the rapid industrialization and urbanization,
excess phosphorus (P) is being discharged into the environment leading to
unintended but ecologically and economically costly consequences such as
eutrophication (Duprey et al., 2016; L€ urling et al., 2016; Zhou et al., 2020).
The occurrence of the hypoxic or “dead” zone in the Gulf of Mexico and
about 400 other locations worldwide is the most salient example of the
damaging effect of eutrophication (Diaz & Rosenberg, 2008; Schindler
et al., 2016; Vonlanthen et al., 2012). Orthophosphate, also known as sol-
uble reactive phosphorus, is the key form of P that can be assimilated by
plants and the other microbes present in water (Kumar et al., 2019). To
curb eutrophication by reducing dissolved reactive P in surface waters, a
broad range of strategies such as adsorption (Kelly Vargas & Qi, 2019; Wu
et al., 2020), chemical precipitation (Huang, Liu, Zhang, et al., 2017), bio-
logical treatment (de Graaff et al., 2020), membrane separation (Nir et al.,
2018), and electrochemical process (Kekedy-Nagy et al., 2020) have been
developed and employed worldwide.
Among these strategies, although biological methods are broadly applied
in the wastewater treatment plants (WWTPs), they are less effective at trace
level, largely due to the presence of insufficient phosphate lowers metabol-
ism of microorganisms (Huang, Zhang, & Li, 2017). In addition, the con-
tamination of pathogens, heavy metals, and toxic organic compounds in
the sewage sludge limit its application for P recovery. Adsorption, however,
is currently the most practical method for removing P from wastewaters,
especially at low P concentration (e.g., below 0.1 mg P L1) (Wu et al.,
2020). Furthermore, adsorption/desorption is a relatively easy process to
recover P from P-containing streams (Bacelo et al., 2020; Loganathan et al.,
2014). Wastewater is rich in P that can be recovered as valuable and useful
nutrient sources. It is reported that theoretically, 15–20% of world demand
for phosphate rock can be satisfied by recovering P from municipal waste-
water alone (Yuan et al., 2012). Therefore, adsorption and recovery of P
from water and wastewater can be viewed as a greener alternative for
industrial and agricultural P consumption.
Phosphorus separation by adsorption during coagulation, followed by
removal through sedimentation and filtration, has been used since the
1950s to treat wastewater using a wide variety of adsorbents (Rittmann
et al., 2011). Although the most common adsorbent used in water remedi-
ation is activated carbon, the relatively complicated production process,
high prices, and expensive regeneration cost of activated carbon restrict its
large-scale application in most developing countries (Hokkanen et al.,
2016). Across many developing countries, only a minor fraction (in some
cases, <5%) of domestic and urban wastewater is treated before its release
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 2025
into the environment (UN-Water, 2019). Even in developed counties, some

studies indicated that advanced technologies are challenging to implement
at many small-scale, rural wastewater treatment plants (Bunce et al., 2018;
Molinos-Senante et al., 2014). Therefore, to achieve the United Nations
Sustainable Development Goal 6 of Clean Water and Sanitation by 2030,
there is a need to develop and apply cost-effective adsorbents with excellent
adsorption and regeneration capacity in the underdeveloped nations
and regions.
The utilization of waste materials as low-cost adsorbents could emphasize
the concept of waste-to-resource supply chains to achieve a circular econ-
omy (Grace et al., 2016; Kushwaha et al., 2013; H. Y. Zhang et al., 2020).
Many industrial wastes contain metal ions (e.g., Ca2þ, Al3þ, and Fe3þ) with
a high affinity for P ions in aqueous solutions (Haynes, 2015). Agricultural
wastes (particularly those containing cellulose, hemicellulose, and lignin)
have abundant surface functional groups (e.g., -OH and -CHO) that can
easily get involved in chemical reactions (e.g., condensation and polymer-
ization), and thus, provide a foundation for agricultural wastes to be con-
verted into some functional polymers (Dai et al., 2018; Tran et al., 2019).
Several valuable studies review and highlight the potential of using waste-
based adsorbents in water treatment (Bhatnagar & Sillanp€a€a, 2010;
Bhatnagar et al., 2015; Mo et al., 2018), although the information about P
removal is scattered and somewhat limited. In a review of three sets of sub-
strates – natural materials, industrial by-products, and man-made products
– for P removal, Westholm (2006) identified the longevity of the sorption
capacity of phosphorus as a research priority. Nguyen et al. (2014) sum-
marized the tradeoffs of modification techniques of agricultural wastes for
enhanced P removal and recovery. Some mostly recent reviews concen-
trated on specific types of adsorbents such as alum sludge (Muisa et al.,
2020) or biochar (Dai et al., 2020; M. Zhang et al., 2020), to elucidate that
modified methods are needed to improve the adsorbent’s performance for
P removal. However, at the present stage, it is still difficult to compare the
P removal capacity among different waste-based adsorbents due to the vari-
ation of experimental condition and potential to make waste-based adsorb-
ents more suitable in a real-world application. Emphasis should be placed
on the waste-based adsorbents end-of-life and improve treatment sustain-
ability, which is often ignored. Therefore, there is a need for “re-review”
the current trends from recent studies by answering three questions: (i)
how to enhance the P removal efficiency, (ii) how to scale up to the prac-
tical level, and (iii) how to achieve sustainable management of the resulting
saturated adsorbents.
Accordingly, in this review, we begin with a summary of the species and
primary pollution sources of P. Then, we synthesize recent developments
2026 H. ZHOU ET AL.
in different waste-based adsorbents used to remove P from wastewater. A

sustainable paradigm of waste-based absorbent is proposed for P removal
that extends beyond immediate benefits to water quality to achieve sustain-
able management of waste-based adsorbents. At last, insights and perspec-
tives are suggested in terms of future research directions and development.
2. Phosphorus forms and major phosphorus pollution sources in water

Phosphorus occurs in waters as different forms, notably soluble forms (e.g.,
<0.45 lm filter) and particulate forms (e.g., retained on a 0.45 lm filter).
Reactive P refers to orthophosphate or more operationally molybdate react-
ive P (MRP), which reflects the widespread use of molybdate in orthophos-
phate colorimetry (Bernhart & Wreath, 1955; Fiske & Subbarow, 1925;
Kitson & Mellon, 1944). The nonreactive P fraction, also known as con-
densed or acid hydrolyzable P (AHP) or organic P (OP), includes inorganic
polyphosphates (metaphosphates and di-, tri-, and tetra-polyphosphates)
(American Public Health Association (APHA) et al., 2012). Among them, it
is widely accepted that the orthophosphate is the key compound respon-
sible for eutrophication and can exist in water as four different species:
H3PO4, H2PO4, HPO42, and PO43, depending on pH conditions
(Kumar et al., 2019). Therefore, orthophosphate is the priority compound
for P removal from water and subsequent recovery of P-rich products.
Nonetheless, recent studies also show the necessity to remove and recover
several types of non-orthophosphates (Lei et al., 2020; Venkiteshwaran
et al., 2018).
Excess P is mostly transported to the soil and water system from
anthropogenic sources. Much of the P that enters the human trophic chain
and is, therefore, last via wastewater sources is ultimately derived from
phosphate rock. Prior to the mid-twentieth century, the majority of P in
the human trophic chain was recycled, from wastes back to croplands in
the form of animal and human manure, with supplementation from guano
deposits (Cordell et al., 2009). Thus, in less than one century, human activ-
ities have effectively quadrupled the flux of P in the biosphere, including
surface waters (Elser & Bennett, 2011). Mekonnen and Hoekstra (2018)
estimated that the global anthropogenic P load to freshwater systems from
both diffuse and point sources was about 1.5 Tg yr1, with 54% of the total
contributed by domestic sector, 38% from agriculture, and 8% from indus-
try, although these relative contributions can vary regionally. For point
sources, one of the most significant P point sources is WWTPs, directly
discharging varying amounts of P into the water. Despite WWTPs being
relatively good at removing P, approximately 10% of the incoming P load
through insufficiently treated wastewater are discharged globally (Desmidt
et al., 2015). For non-point sources, agriculture is the main contributor of

P transfer to surface waters. In agricultural systems, P inputs in the form
of concentration P fertilizers and/or manure are added to support crop
production (Hopkins & Hansen, 2019). Still, the majority of these P inputs
accumulate in the soil as residual P, accumulation of which over multiyear
to decadal timescale is known as legacy P (Rowe et al., 2016). Each year,
almost 35% (6.30 ± 3.20 million metric tons) of P fertilizer are transferred
from soil to the surface waters through surface runoff (Cordell & White,
2014) with around 75–90% P that is transported with runoff water from
cultivated land is in particulate form (Sharpley et al., 2003). Meanwhile,
urban non-point source P pollution is increasing with urbanization, and
urban non-point source pollution can be a severe threat to proximate
urban watersheds as well as regional watersheds not in the urban area.
Eventually, P contained in the municipal, domestic, and agricultural waste-
water could be transported from wastewater plants, wetlands, enveloped tile
drains, subsurface tile drains, among other sources, into the surface waters.
Therefore, these human-made points of solid and liquid P-rich wastes are
the outlets and pollution sources of P, to which adsorbents can be targeted
to intercept P-rich waste streams for subsequent P removal.
Table 1 summarizes highly variable P concentrations by diverse waste-
waters originating from industrial, agricultural, and urban sources.
According to the United States Environmental Protection Agency (USEPA),
the total phosphorus (TP) should not exceed 50 lg L1 if the water is dis-
charged directly into lakes or reservoirs (USEPA, 1986). Further, more
stringent water quality goals and standards as low as 5–10 lg L1 TP have
been established in ecologically sensitive U.S. zones like the Great Lakes
and Everglades (USEPA, 1998; Venkiteshwaran et al., 2018). Clearly, given
relatively high P enrichment, most wastewater effluent still has the potential
to trigger eutrophication (Table 1) and is a priority target for decreasing
point source contributions of P to surface waters.
3. Waste-based absorbents for phosphorus pollution control

The waste-based absorbent is a general term for the absorbent that is syn-
thesized, derived, and manufactured from waste materials. The waste-based
adsorbents investigated in this study have been broadly classified into four
categories: industrial waste-based adsorbents (IWAs), agricultural waste-
based adsorbents (AWAs), construction and demolition waste-based
adsorbents (CDWAs), and marine debris-based adsorbents (MDAs). In this
section, we also discuss critical concerns of practical considerations that
need to be addressed for successful implementation.
2028 H. ZHOU ET AL.
Table 1. P concentrations reported in wastewater from different sources.

Wastewater type PO43– (mg-P L1) Ref.
Phosphating wastewater 103 ± 4.30 Huang, Zhang, Yang, et al. (2017)
Microbial fuel cells wastewater 1460 ± 15.0a Huang, Huang, Liao, et al. (2017)
Treated municipal sewage 0.441 ± 0.380 Drenkova-Tuhtan et al. (2017)
Rural domestic wastewater 103.6 ± 6.90a He et al. (2017)
Toilet Wastewater 56.9 Cid et al. (2018)
Dairy wastewater 28.5a Rabinovich et al. (2018)
Wastewater from cytidine monophosphate industry 1500 Yang, Sheng, et al. (2019)
Raw swine wastewater 97.4 ± 30 Wang, Wei, et al. (2019)
Fish processing wastewater 180 Trivedi et al. (2019)
Industrial textile wastewater 83.2–95.4 Pazdzior et al. (2019)
Starch wastewater 28.5a Du et al. (2019)
Secondary wastewater effluent 7.80 Pap et al. (2020)
Wastewater from anodizing industry 4336 Delgadillo-Velasco et al. (2020)
Human urine 917 ± 20.2 Pinatha et al. (2020)
Pulp mill wastewater 3.70a Bentancur et al. (2020)
Electro-plating wastewater. 7.37–12.6a Li, Dong, et al. (2020)
Industrial effluent 11.7 Noubli et al. (2020)
Reclaimed wastewater for irrigation 1.90 ± 0.460a Mclennon et al. (2020)
Post-hydrothermal processing wastewater 326 Crossley et al. (2020)
Indicates total P (mg-P L1).
a
3.1. Industrial waste-based adsorbents

Industrial waste-based adsorbents are developed from various industrial
residues, which generate during industrial processes. Here, we focus on the
recent activities – within the last five years – in the development of com-
mon industrial waste products for P removal. The detailed comparisons
regarding different industrial waste-based adsorbents are presented in
Table 2.
Coal fly and bottom ash, two primary groups of coal ash produced mil-
lions of tons annually during the coal combustion process, have been
widely studied as a low-cost alternative for the removal of P. Normally,
Coal fly ash is 65–95% of the total ash generated. In China, more than 600
million tons of CFA was produced in 2015 (Ding et al., 2017). The fly ash
pellets manufactured by Li et al. (2018) showed relatively stable P removal
efficiency of 68–75% in a lab-scale horizontal-flow bioreactor and could be
incorporated into an edge-of-field practice. Further, Zhou et al. (2019)
compared the P adsorption capacity of fly ash pellets (Qm 2.05 mg P
g1) and bottom ash pellets (Qm 2.56 mg P g1), indicating the bottom
ash pellets was more suitable adsorbent than fly ash pellets due to higher P
adsorption capacity, and also exhibited lower leaching of trace metal ele-
ments of human health concern (e.g., cadmium).
Red mud (bauxite residue, RM) is an alkaline byproduct of alumina
extraction via the Bayer process. Each year, about 90 million tonnes of red
mud are produced globally (Wang et al., 2008). In recent years, a particular
focus has been placed on how to develop novel red mud-based adsorbent
and examine its feasibility in practical application (Cusack et al., 2018; Si
et al., 2017). Cusack et al. (2019) conducted rapid, small-scale column tests
Table 2. Presentation and evaluation of industrial waste-based adsorbents.
Maximum
Waste- Sorption capacity
based absorbents Modification method (mg g–1) Limitation Water samples Ref.
Fly ash pellets Thermal modified with 0.0590–0.114 Heavy metals leaching; Detention pondb Li et al. (2018)
lime/ clay Poor saturation time
Bottom ash pellets Thermal modified with 2.56 Possible desorption condition; Synthetic solutiona Zhou et al. (2019)
lime/clay Field studies are needed
b
Red mud Red mud 0.0450–0.270 Metal leaching potential, Agricultural waters Cusack et al. (2019)
especially for Al and Fe.
Red-mud based Pelleting process 0.420 Limited information on the Synthetic watera Shabnam et al. (2019)
ceramic media elements leaching
a
Thermally treated Thermal treatment – High energy cost in Synthetic water Lin et al. (2020)
red mud thermal treatment
Rapid cooled basic Mixed with sand 3.60 Limited information on the Synthetic solutionb Park et al. (2017)
oxygen furnace slag elements leaching
a
Porous calcium Hydrothermal synthesis 3.77–11.3 High pH of outflow Synthetic solution Fang et al. (2018)
silicate hydrate
Alum- and iron- Aeration and chlorination to 30.3–47.6 Dewatering of sludge is needed Synthetic/ secondary Bal Krishna et al. (2016)
a
based sludge remove iron effluent wastewater
Urban sewage Pyrolysis þ Dolomite 29.2 Powder form biochars are Synthetic solutiona Li et al. (2019)
sludge biochar difficult to collect
and transport
Urban dewatered Alkaline 93.9 Reusability of the adsorbent Synthetic solutiona Li, Li, et al. (2020)
sewage sludge La- treatment þ Pyrolysis can’t be evaluated accurately
coated biochar due to the mass loss during
solid–liquid separation
a
Indicates batch experiments.
b
Indicates column tests including constructed wetland and continuous-flow experiments.
2029
2030 H. ZHOU ET AL.
to predict the P removal capacity of RM in both low (forest runoff) and

high (dairy soiled water) range P-concentrated waters. Shabnam et al.
(2019) designed an RM-based ceramic medium (RMCM), making it suit-
able for practical applications in a built environment as well as promoted
biomass (Iris latifolia) growth. Lin et al. (2020) found the thermal treat-
ment of RM caused significant changes in chemical composition, morph-
ology, and surface property, leading to a different performance in
phosphate removal. Thermal treatment of RMs brought about mineral
decomposition and phase transformation, which in turn altered the surface
acidity and the mineral (aluminum and calcium ions) leachability of RMs.
Slag, including blast furnace slag, basic oxygen furnace slag, and electric
arc furnace slag, has long been used in agricultural best management prac-
tice and could remove appreciable amounts of dissolved P compared to
traditional sand media (Penn et al., 2020). China produces approximately
120 million tons of slag per year. Also, in the EU, with a primary steel pro-
duction of about 110 million tons, this leads to 10 million tons of slag
annually (EUROFER, 2018). Blast furnaces are used for iron production,
whereas electric arc furnaces and basic oxygen furnaces are used for steel
production (Proctor et al., 2000). The rapid cooled basic oxygen furnace
slag (RC-BOFS) generated from a new economical and environmentally
friendly slag process (Baosteel Slag Short Flow) (Wang & Chen, 2016).
Park et al. (2017) reported that RC-BOFS had a nearly 95% P removal rate.
They also predicted the addition of a 25% RC-BOFS to the coarse sand
could significantly increase the longevity of constructed wetland up to
3 years. Carbide slag is a byproduct of hydrolysis of calcium carbide (CaC2)
for the production of acetylene. Fang et al. (2018) developed a novel porous
calcium silicate hydrate derived from carbide slag through hydrothermal
synthesis (Figure 1). The resultant material exhibited distinct skeletal struc-
tures and pores and was rich in Ca-OH functionalities. Once releasing
Ca2þ and OH into phosphate wastewater, the dissolved P is precipitated
as whitlockite (Ca3(PO4)2) and hydroxyapatite (Ca5(PO4)3OH). P can also
diffuse through the mass transfer to the modified carbide slags’ surface and
react directly with Ca-OH groups.
Diverse sludge generated from water and wastewater treatment plants,
despite their characteristics could be varied, were shown to efficiently
remove P from wastewater. Water treatment sludge (WTS) generated from
the addition of alum (Al2(SO4)314H2O) or ferric chloride (FeCl3) during
the coagulation process (Rebosura et al., 2020; Xu et al., 2020). Bal Krishna
et al. (2016) showed, under the secondary effluent wastewater condition,
the maximum adsorption capacity of iron-based sludge predicted by
Langmuir model was 32.3 mg g1, while the lowest experimental adsorption
capacity observed of alum-based sludge was 40.0 mg g1. However, this
Figure 1. Hydrothermal synthesis of P-CSH derived from carbide slag and proposed mechanism
on phosphate removal from wastewater.
contradicted some earlier studies (Genz et al., 2004; Gibbons & Gagnon,
2011), may be due to variations in sludge composition, which originated
from different unit treatment processes and water qualities.
Furthermore, converting organic industrial wastes into functional bio-
chars with thermal treatment can reduce the leaching of heavy metals,
organic pollutants, and pathogens from sludge products into soil and water,
especially for sludge wastes (Chen et al., 2020; Xia et al., 2020). Li et al.
(2019) developed innovative biochar derived from urban sewage sludge by
doping dolomite. Acidic conditions favored the P removal with biochar,
exhibiting high P removal efficiency of 96.8%. Further, J. Li et al. (2020)
reported a high P adsorption capacity of 93.9 mg g1 determined by
Langmuir isotherm model was achieved by lanthanum (La)-coated biochar
obtained from urban dewatered sewage sludge. The La-coated biochar
showed high adsorption capacity as the solution pH varied from 3.0 to 6.0
and was insensitive to the coexisting chloride, nitrate, sulfate, bicarbonate,
and citrate.
3.2. Agricultural waste-based adsorbents

Agricultural waste entails a wide range of organic materials discarded by
human beings in crop production and forestry such as plant waste, agricul-
tural and sideline products processing waste, rural household waste.
2032 H. ZHOU ET AL.
Through thermal or chemically modifying properties of agricultural waste

to manufacture agricultural waste-based adsorbents, the sorption capacities
of agricultural waste can be improved. Thus, with a growing number of
agricultural wastes are developed as adsorbents for contamination treat-
ment (Table 3), we described the most representative research to illustrate
the latest development of agricultural waste-based adsorbents for
P removal.
For the agricultural wastes originating from croplands, raw wastes modi-
fied by different chemical treatments is a mainstream strategy to produce
agricultural waste-based adsorbents. Of particular interest, metal loading
and amine-grafting have been widely used to increase the P adsorption cap-
acity of these organic matter-based adsorbents. For example, okara is the
pulp leftover from soybeans after the beans are pressed for soy milk. For
every 1 kg of soybeans used in manufacturing soybean curd, about
1.10–1.20 kg of okara is obtained. The amount of okara generated by the
soybean curd-manufacturing sector is about 800,000 tons in Japan, 310,000
tons in Korea, and 2,800,000 tons in China (Vong & Liu, 2016). Nguyen
et al. (2015) produced a Zr(IV)-loaded adsorbent from raw soybean residue
(okara). In column tests, the maximum dynamic adsorption capacity for P
was estimated to be 16.4 mg g1, at pH 3. However, a decline in P adsorp-
tion was observed in alkaline conditions (pH ¼ 8). Taking a different
approach, Pan et al. (2020) reused biogas residue as a host to anchor qua-
ternary-amine groups, forming the amine-functionalized adsorbent based
biogas residue (BR-N; Figure 2). In the batch study, the BR-N showed
excellent removal capacity for both P and nitrate across a wide pH range
of 5.00–9.00. The maximum adsorption capacities of BR-N was 34.4 mg P
g1 for phosphate and 64.1 mg g1 for nitrate, and even after continuous
eight cycles of adsorption-desorption, BR-N still exhibited >82.0% adsorp-
tion capacity for P and N removal. Physicochemical characteristics revealed
that BR-N has abundant quaternary-amine groups to enhance the diffusion
and electrostatic attraction of P. Further, in column tests to remove P and
N from actual surface water and simulated solution, BR-N removed not
only N and P in the multicomponent water body but also reduced turbidity
(lower than 3.50 NTU in effluent).
Eggshell is a kind of agricultural waste produced at large amounts by
eggprocessing industries. Global egg production for the year 2018 was 78
million metric tons, contributing approximately 8.58 million metric tons of
eggshells which are being discarded mostly as waste (Waheed et al., 2020).
Panagiotou et al. (2018) found the adsorption capacity of calcined eggshells
increases as the calcination temperature increases and inversely to particle
size. The specific surface area of calcined eggshells increased from 0.310 to
1.57 m2 g1 as the calcination temperature raised from 600 to 900 C. The
Table 3. Presentation and evaluation of agricultural waste-based adsorbents.
Maximum
Sorption capacity
Waste-based absorbents Modification method (mg g–1) Limitation Water samples Ref.
Zr(IV)-loaded okara NaOH treatment þ Zr load 16.4 Some organic matters and Synthetic solution þ real Nguyen et al. (2015)
b
chloride were released into municipal wastewater
the solution
Biogas residue Amine-gifting 34.4 Improper disposal of depleted Synthetic solution þ practical Pan et al. (2020)
based biosorbent biosorbents would cause surface waterab
serious pollution
Calcined egg shells Calcination (600 Cfor 4 hr, 7.90 31.7 Potential harmful substances Synthetic solution /anaerobic Panagiotou et al. (2018)
800 Cfor 2 hr, and 900 C should be eliminated digester effluenta
for 30 min
Al-eggshell Dried egg shell immersed in 3.80 Further optimization on Synthetic solutiona Zhang et al. (2018)
AlCl3 solution for 24 hr processing conditions
is required
La(OH)3-modified Pyrolysis (300 C) þ magnetic 101 Relatively high Synthetic solutiona Liao et al. (2018)
magnetic modification þ La(OH)3- production cost
pineapple biochar modification
CaO-biochar composites 800 Cat a heating rate of 5 C/ 231 Possible desorption condition Synthetic solutiona Liu et al. (2019)
prepared from min under N2 atmosphere
eggshell and rice straw
Al/Mg- modified biochar Pyrolysis (600 C) þ immersed 152 Further studies are required to Synthetic solutiona Yang, Zhang, et al. (2019)
in scale up to practical level
MgCl2 and AlCl3 solution
Fe/Al Pyrolysis(500 C) þ immersed 180 – 215 Synthetic solutiona Peng et al. (2019)
(Hydr)oxides-Biochars into FeCl3 and AlCl3
a
b
Indicates column tests.
ab
Indicates both batch and column tests were conducted.
2033
2034 H. ZHOU ET AL.
Figure 2. (a) Scheme of the preparation of BR-N form the virgin biogas residue; (b) A strong
electrostatic force between NþCH2CH3)3 and H2PO4 than NO3–; (c) High recoverability of phos-
phate-laden BR-N.
eggshell calcination at 900 C for 30 min resulted in 55% and 95% P

removal after 1 and 24 hr, respectively. The Al-coated eggshell (Al-egg
shell) prepared by Zhang et al. (2018) showed an approximately threefold
increase in the surface area (SBET ¼ 20.8 m2 g1) compared with the nat-
ural eggshell (SBET ¼ 6.00 m2 g1) and resulting in a better P adsorption
capacity. However, the authors also indicated that no aluminum hydroxide/
oxide peak information was found from the XRD patterns, the mass of Al
was too small, or aluminum hydroxide/oxide XRD diffraction peak is wide
could be the plausible reasons to explain the phenomenon.
Biochar derived from pyrolysis of various agricultural waste (biomass) is
another treatment approach that yields a highly porous structure with
abundant organic functional groups (Krishna Veni et al., 2017; Zhong
et al., 2019). To further enhance P removal, doping biochars with metal
cations (Ca, Fe, Mg, Al, La, etc.) is the most common modification method.
Liao et al. (2018) shown the La(OH)3-modified magnetic pineapple biochar
(pyrolysis of pineapple peel at 300 C) exhibited excellent P adsorption cap-
acity up to 101.2 mg g1 and with high removal efficiency (>96%) . Liu
et al. (2019) produced CaO-biochar composites, and a maximum adsorp-
tion capacity of 231 mg g1 could be obtained through a mixed sample that
was prepared from the eggshell and rice straw with a mass ratio of 1:1.
Layered double hydroxides (LDHs) are composed of positively charged metal
hydroxide layers, including the divalent cation (Fe2þ, Mg2þ, Ni2þ, and Mn2þ)
or trivalent cation (Fe3þ, Al3þ, and Cr3þ) and the interlayer anion (CO32,
SO42, OH, and Cl) along with water molecule (Yang, Zhang, et al., 2019).
Immense interests have shown by scientists to assemble LDHs with biochar to
manufacture mineral-biochar composites, and the resulting biochar/LDH com-
posites exhibit significant improvement in the physicochemical and adsorption
characteristics (Peng et al., 2021). Yang, Zhang, et al. (2019) prepared Al/Mg-
modified biochar (feedstock: corn stalks biomass) with a P adsorption capacity
of 152 mg g1. In another study, Peng et al. (2019) applied response surface
methodology (RSM) to optimize the production of synthesized Fe/Al
(Hydr)oxides-Biochars (feedstocks: almond shell, corn stalk, and dairy manure)
for the P removal. These Fe/Al (hydr)oxides-Biochars presented excellent P
adsorption capacities (ranged from 180 to 215 mg P g1) due to a good
amount of surface area, pore volume, and reactive surface hydroxyl sites.
All of these studies above indicated agricultural waste-derived biochar
could be low-cost, environment-friendly, and effective adsorbent for phos-
phate removal. However, the modification methods by impregnating bio-
chars with metal ions may require a large amount of reagent with
cumbersome loading procedure and be time-consuming, which leads to an
increase in the expense of the final material. Alternatively, Jun and Ahn
(2016) have proposed a rapid (10 min) method for Mg deposition to elec-
trochemically activate biochar produced from Laminaria japonica, brown
marine macroalgae, for greater porosity. After modification, the specific
surface area of biochar was increased up to 56.4 m2 g1, while the raw bio-
char has poorly structured porosity (2.39 m2 g1).
3.3. Construction and demolition waste-based adsorbents

Construction and demolition wastes (CDWs) are the unwanted materials pro-
duced from the construction industry, such as brick and concrete. Since the
construction industry is a significant consumer of natural resources, nearly 2.65
billion tons of CDWs generated annually (Tam et al., 2018). Although landfill-
ing is widely adopted for CDWs disposal, it is facing increased challenges
attributable to land space restriction and growing concerns of contamination.
Several studies have focused on the recycling of this waste to fabricate engineer-
ing materials, such as recycled aggregates concrete and composite material
(Sormunen & K€arki, 2019). However, a recent study reported that only 1–2%
of CDWs are recycled (Hoang et al., 2020). Thus, there is an abundant supply
of these waste materials and in close proximity to urban point sources of P
losses. Recycling it as adsorbent is regarded as a win–win fix in environmental
protection and waste management (Liu, Zhu, et al., 2020).
Saeed et al. (2018) observed a high P removal (89%) from industrial
wastewater in a hybrid system packed with recycled brick due to the
2036 H. ZHOU ET AL.
adsorption process. Bao et al. (2020) found the autoclaved aerated concrete par-
ticles (AACPs) from construction waste were more efficient (72%) than com-
mercially available ceramsite (34%) in removing P from domestic wastewater.
Liu, Zhu, et al. (2020) demonstrated the P removal ability of waste concrete
powder increased with decreasing particle size (in the range of 1.07–4.96 mg P
g1). The smaller particle size fraction (1–100 mm) of waste concrete powder
had more Ca-rich and porous hardened cement paste powder, resulting in
higher P bonding capacity. A study by Liu, Quan, et al. (2020) developed Ca-
rich cement mortar from waste concrete (CCMs), the P adsorption capacity of
modified CCM reached 100 mg g1, and the P concentration in wastewater can
be reduced from 100 mg L1 to below 0.1 mg L1 within 30 min. dos Reis
et al. (2020) thermally treated an inorganic sludge from the inert part of con-
struction and demolition wastes at 800 C for 2 hr, obtained a 140% greater P
adsorption capacity of 57.6 mg g1 compared to the unmodified sludge
(24.0 mg g1). Detailed information is summarized in Table 4.
3.4. Marine debris-based adsorbents

Marine debris consisting of items that have been made and used by people
are deliberately or accidentally discarded into the sea or rivers or on
beaches. Different kinds of shells (e.g., oyster shell and gastropod shell) are
marine debris discard by the aquaculture sectors with emerging potential
for use as P adsorbents (Table 5). The world production of oyster shells is
estimated to nearly 3.90 million metric tons, which leads to a real environ-
mental issue (Bonnard et al., 2020). Martins et al. (2017) demonstrated that
oyster shell waste is a highly efficient adsorbent for P removal in seawater,
particularly after calcination at 900 C for 3 hr. Oyster-shell calcination
boosted P removal (95%) from saltwater after 15 min. In a similar
approach, Paradelo et al. (2016) found that the calcined shell had a higher
P retention capacity than a non-calcined shell due to the conversion of ara-
gonite to calcite and calcium carbonate to calcium oxide during calcination.
Romar-Gasalla et al. (2016) also found that the mussel shell ash showed
the highest P retention capacity, reaching >95%. To achieve very low con-
centrations of P, Yin et al. (2020) prepared a metal-modified mussel shell
by polyaluminium chloride, Fe(OH)3, and La2O3. Long-term efficient
removal of P (<0.1 mg L1) was achieved during a 3-month removal
experiment of P-contaminated water. Sun coral was also used as an adsorb-
ent for P removal in synthetic and real wastewater (Vianna et al., 2016).
Chitosan, which can be extracted from fishery wastes (shellfish, shrimps,
crabs, and insects), is the second most naturally abundant polymer after
cellulose. Chitosan-based adsorbents have been extensively and successfully
applied, but the adsorbed pollutants may be leached to the environment
Table 4. Presentation and evaluation of construction/demolition waste-based adsorbents.

Waste- Maximum
based Modification Sorption capacity Water
absorbents method (mg g–1) Limitation samples Ref.
Recycled brick Packed with – Post-treatment Industrial Saeed
sugarcane and disposal wastewaterb et al. (2018)
bagasse are required
Autoclaved Autoclaved at a – Limited Domestic Bao et al. (2020)
aerated saturated information wastewaterb
concrete steam on the
particles pressure elements
of 180 C leaching
Waste concrete Thermal 1.10–5.00 Affected by pH Synthetic Liu, Zhu,
stress and potential solutionb et al. (2020)
method high pH
Modified waste Heat treatment 100 of outflow Synthetic Liu, Quan,
concrete (800 Cfor solutiona et al. (2020)
powder 20 min) or
HCl
(5.0 mmol
g–1)
Construction Thermally 57.6 Desorption and Synthetic dos Reis
and treated at the presence solutiona et al. (2020)
demolition 800 C of heavy
wastes for 2 hr metals must
sludge be addressed
a
b
Indicates column tests including constructed wetland and continuous-flow experiments.
after adsorption (Wang & Zhang, 2017). At the current stage, most studies
used commercial chitosan to develop chitosan-based adsorbents because of
its low price (Jang & Lee, 2019; Yang, Li, et al., 2016), and more than 1.2
million tons of crustacean shells were processed into chitin around the
world annually (Mo et al., 2018). Recently, Pap et al. (2020) proposed a
low-cost and low-temperature synthesis methodology to produce chitosan-
calcite adsorbent from the raw carapace (crustacean exoskeleton) and used
for P removal from secondary wastewater effluent (Figure 3). The max-
imum P adsorption capacity was 21.4 mg g1 (at 22 C), and the endoder-
mic process reached equilibrium after 120 min. The pH had a significant
influence on P adsorption mechanisms and capacity. Material characteriza-
tion (SEM/EDX micrographs) demonstrated the disappearance of the potas-
sium (K) peak in the P-loaded sample, likely reflecting a reaction between
the monovalent anion H2PO4 (on the surface) and K to form potassium
dihydrogen phosphate (Uzunova & Mikosch, 2016).
3.5. General consideration

Four types of waste-based adsorbents used for P pollution control are pre-
sented in this section. Such wastes are low-cost and available in large quan-
tities, and modifying their physicochemical properties can enhance
adsorption capacity for more effective phosphate removal from wastewaters.
2038
H. ZHOU ET AL.
Table 5. Presentation and evaluation of Marine debris-based adsorbents.

Maximum
Waste-based Sorption capacity
absorbents Modification method (mg g–1) Limitation Water sample Ref.
Calcined oyster shell Calcination at 900 C – Affected by pH Artificial seawatera Martins et al. (2017)
for 3 hr and potential high
Calcined mussel shell Calcination at 550 C – pH of outflow Synthetic solutionab Paradelo et al. (2016)
for 15 min
Metal-modified Thermally treated at 600 C for 101, 56.5, and 91.7 Limited information Synthetic solution/real Yin et al. (2020)
mussel shell 2 hr þ immersed in on the environmental
Fe(OH)3, La2O3, and elements leaching watera
PAC solution
Chitosan- Thermochemical modification 21.4 Further optimization Synthetic solution/ Pap et al. (2020)
calcite adsorbent with deacetylation of the would be needed secondary
chitin chain in the presence before an industrial wastewater
of potassium scale application effluentab
hydroxide (KOH)
a
ab
Indicates both batch and column tests were conducted.
Figure 3. The synthesis pathways and P adsorption mechanism of chitosan-calcite adsorbents:

(a) Schematic diagram of chitosan-calcite adsorbent fabrication process; (b) SEM/EDX micro-
graphs before and after P adsorption; (c) Schematic of proposed adsorption mechanisms of P
onto chitosan-calcite adsorbents.
Besides, past studies have evaluated the performance of waste-based adsorb-

ents under diverse experimental conditions (e.g., real wastewater and col-
umn tests condition). This is a crucial step to provide reliable information
for the actual application of waste-based adsorbents. However, several limi-
tations are also demonstrated above regarding the use of waste-based
adsorbents. Particularly, the environmental concerns and economic evalu-
ation are two key factors for waste-based adsorbents for P removal. Herein,
we provide several critical comments on these two aspects.
3.5.1. Environmental concerns

Industrial and municipal waste products can present several potential envir-
onmental risks. Coal ash and red mud may release excessive concentrations
of trace metal(loid) elements to the aquatic ecosystems. Even for agricul-
tural waste products, in order to obtain high P removal capacity, several
modification methods may induce environmental risk (Nguyen et al.,
2014). Some solutions have been proposed to avoid secondary pollution.
The first solution is to immobilize the heavy metals into the wastes. To this
end, thermal modification is an effective immobilization treatment, as
reviewed in detail by Guo et al. (2017). However, variation in the physical
and chemical properties of the wastes means that there is not yet a consen-
sus on the temperature setting during the high-temperature modification
process, which would affect the energy consumption and manufacture cost.
The second solution is to exploit the derived pollution to treat pollution.
2040 H. ZHOU ET AL.
For instance, slags release large amounts of OH and Ca2þ into the water
body. Under this circumstance, slag could be used to treat wastewater (e.g.,
mining wastewater), which contains significant amounts of Hþ, sulfate
(SO42), and various toxic metals. It is highly possible that Hþ in mining
wastewater is buffered with OH, and SO42 is precipitated with Ca2þ to
form CaSO4 (Yang et al., 2018). Therefore, prior to use, it is crucial to
understand the environmental impact of waste-based adsorbents and imple-
ment proper management practices to minimize risk.
3.5.2. Economic evaluation

A well-known advantage of reusing waste material for P removal is that, by
virtue of being wastes, these adsorbents are relatively low in costs compared
to other adsorbent feedstocks. However, it is noteworthy that “low-cost”
adsorbents refer to the raw material. Various factors, such as manufactur-
ing cost, geographical locations, transportation logistics, marketing manage-
ment, both recycle and lifetime issues, should be fully considered. For now,
relatively little is known about such information of waste-based adsorbents
P removal processes in the existing literature. Pap et al. (2020) calculated
the production cost of chitosan-calcite adsorbent developed from seafood
waste to be 0.561 USD kg1 (561 USD ton1). Using this price, the adsorb-
ent mass required, calculated adsorption capacity and treated effluent vol-
ume, the cost of treatment would be approximately 17 USD m3 or
approximately 26 USD kg1 P for a high P concentration effluent (i.e.,
1–2 mg P L1; qe,1–2 mg L1¼ 21.3 mg g1) and approximately 4 USD m3
or approximately 637 USD kg1 P for a low concentration effluent. This
price is much lower in comparison to ‘classic’ activated carbon filtration of
treated wastewater (50–200 USD m3), or for reverse osmosis (100–450
USD m3), ion exchange, or electrolysis (Gupta et al., 2012), and other P
filtration processes (269 USD kg1 P) (Bashar et al., 2018). Li et al. (2019)
calculated the total cost of the dolomite-modified sewage sludge biochar
when the modified biochar dosage was 2.20 g L1, the P removal efficiency
observed to be approximately 95%. Under this condition, the total cost of
P removal by the dolomite-modified biochar is estimated to be 1.76 USD
kg1 P, which comprises the costs from sewage sludge disposal (0.0300
USD kg1), biochar preparation (0.290 USD kg1), and saturated biochar
application (0.100 USD kg1). Considering the commercial activated car-
bons normally cost more than 3.00 USD kg1, modified biochars usage is
economically viable. Notably, in some cases, although the price of a specific
adsorbent is higher, if the adsorbent can be reused several times and the
regeneration process is convenient and inexpensive, this waste material still
could be considered as an economical adsorbent. The regeneration cost
should also be considered in the overall cost of the process. For instance,
in an economic analysis of regenerating unmodified and modified absorb-

ents conducted by Ajmal et al. (2020), the production costs of modified
adsorbents were higher than the unmodified materials, but the overall pro-
cess cost can be greatly compensated by the higher phosphate removal and
strong reusability potential. As a result, modified adsorbents are more eco-
nomical (107–117 USD mol1 P) than unmodified materials (187–216 USD
mol1 P). To explore additional potential waste materials and/or their
modification for enhanced P removal or field-use properties, economic
evaluation is, thus, essential for waste-based adsorbent to move forward to
practical application.
3.5.3. Selection criteria of waste-based adsorbents

Careful selection of waste-based adsorbents can lead to significant enhance-
ment of the P removal efficiency. The proposed selection criteria should
not only consider wastes with high P removal capacity but also the feasibil-
ity and sustainability of engineering utilization. Distilling takeaways of pre-
vious studies with practical knowledge, we propose that eight criteria need
to be met: (1) low feedstock cost; (2) geographical availability; (3) sufficient
quantities; (4) technically engineering; (5) limited secondary pollution; (6)
physical properties conducive to flow-through: particle size distribution,
hydraulic conductivity, porosity, and bulk density; (7) durability; (8) readily
replacement.
4. A sustainable paradigm for waste-based absorbent in P

pollution control
To date, scientists are not just simply seeking to improve the adsorption
capacity of waste-based adsorbents; they are also interested in achieving
sustainable management of waste-based absorbents during and after the P
removal process. Valorization of P-rich wastes generated from wastewater
or agricultural runoff treatment can amplify the economic incentives for
removing P (Hertzberger et al., 2020; Margenot et al., 2019; Trimmer &
Guest, 2018). P recovery from saturated waste-based absorbents is a fasci-
nating option and being proposed as a way to advance the United Nations’
sustainable development goals, notably food security, and sustainable man-
agement of water (Trimmer et al., 2017, 2019). This systems approach to
valorizing the P removed – also known as a circular P economy –
addresses historically overlooked constraints to achieve sustainability reduc-
tions of P. Here, we expound various strategies and insights incorporated
into the waste-based absorbent P removal treatment for maximizing the
treatment’s sustainability and valorization. The schematic process is shown
in Figure 4, which provides a wholistic diagram for production –
2042 H. ZHOU ET AL.
Figure 4. The sustainable pathway of waste-based adsorbents in phosphorus pollution con-

trol processes.
application – recovery – regeneration – disposal of waste-based adsorbents

for a sustainable P pollution control practice.
First, producing waste-based adsorbents with excellent performance is
vitally important to achieve sustainable waste management. According to
the selection criteria of waste-based adsorbents, under the suitable modifi-
cation methods, different waste-based adsorbents can be developed to
improve the P pollution control efficiency, reduce utilization cost, and min-
imize environmental impacts. The modification methods have been intro-
duced in Section 3 as examples.
Second, the application of these waste-based adsorbents should follow
the wastewater treatment goals and take the specific water quality charac-
teristics into account. So far, the majority proportion of waste-based
adsorbents are applied as substrates or filter materials in P removal struc-
tures, such as constructed wetlands, agricultural ditches, and subsurface
drainage. It is widely accepted that different types of waste-based adsorb-
ents could be combined and contained in a complete P removal unit in
order to gain a higher P removal efficiency. Many researchers in the
United States, Europe, and Canada have utilized steel slag and acid mine
drainage treatment residuals as substrates for removing dissolved P from
domestic wastewater (Penn & Bowen, 2017). More importantly, there has
been growing interest in capitalizing on synergies among various waste-
based adsorbents to improve multipollutants simultaneous removals cap-
acity. For instance, a combination of woodchip bioreactors with recycled
steel byproduct filters (Goodwin et al., 2015; Hua et al., 2016) or fly ash
pellets (Li et al., 2018) was able to remove both N and P from water. The
woodchip bioreactors have demonstrated N removal efficiencies up to
100%, and the recycled steel byproduct or fly ash pellets can effectively
remove P from effluents. A series of agricultural waste (e.g., rice husk and
potato peel) have an advantage as versatile adsorbents in absorbing inor-

ganic and organic contaminants (Bhatnagar & Sillanp€a€a, 2010; Dai et al.,
2018). Wang, Zhao, et al. (2019) indicated the constructed wetlands with
walnut shell enhanced the denitrification process and could achieve prefer-
able purification of TP (80.3%), TN (51.8%), COD (97.4%), and NH4þ-N
(98.8%), respectively, at middle and high influent pollutant loadings.
Third, the recovery of P from the waste-based adsorbents and utilizing it
as soil fertilizers can provide benefits beyond the P removal. Elution and
direct use are the two most studied approaches to recover P from adsorb-
ents. Bacelo et al. (2020) concluded the NaOH solution is the most appro-
priate eluent used for P desorption. This phenomenon can be explained by
the OH ions of the eluent exchange with the attached phosphate ions.
The desorption percentage provided by NaOH solutions generally increases
with concentration until equilibrium. Yang, Jin, et al. (2016) developed a
tablet precipitation material (TPM) from used white cement, the maximum
recovery capacity achieved was 3.81 ± 0.240 mg g1. Chen et al. (2018) have
shown the adsorption capacity of agricultural waste (cow (Bos taurus)
dung-derived engineered biochar) reached 345 mg g1 and acted as an
excellent slow-release fertilizer in promoting the seed germination, growth,
yields, and P concentration of lettuce (Lactuca sativa). Leng et al. (2019)
indicated the meat bone meal incineration ash after wastewater treatment
was obtained with a P content of 16.2 ± 0.120% (or 37.1 ± 0.270% P2O5),
higher than P content of commonly seen natural phosphate rock (15.3% P
or 35% P2O5), and the acid consumption for P recovery from the P-satu-
rated ash was reduced by 20% compared with the original ash. Apart from
recycling as P fertilizer, many industrial and agricultural waste amendments
have beneficial effects on crop growth and disease resistance (Anyaoha
et al., 2018; Han et al., 2019). For example, steel slag with rough surface
textures and loose porous structure mainly comprises silicon, calcium, iron,
and potassium, which is beneficial to increase soil microbial activity of
methanotrophs and the nutrient content (organic carbon, and total nitro-
gen) in soil (Das et al., 2019; Wang et al., 2014). Accordingly, choosing the
appropriate spent waste product can deliver cost-effective remediation tech-
niques and fulfill “green and sustainable remediation” principles.
Fourth, the regeneration of waste-based adsorbents for continued P
removal can reduce the cost of media replacement. Currently, biochars
derived from agricultural and industrial wastes represent good examples of
P removal from wastewater and subsequent regeneration. Xu et al. (2019)
developed La-biochars (lanthanum doped biochars derived from lignocellu-
losic wastes) with a high phosphate adsorption capacity of 36.1 mg P g1,
presenting excellent reusability with 92% desorption efficiency and retained
85% adsorption capacity after five recycle. This type of La-biochar material
2044 H. ZHOU ET AL.
could be applied as a sustainable building block for the preconcentration of

P for efficient pollutant purification. Kizito et al. (2017) shown that the
maximum P adsorption (at initial 150 mg L1) of four slow pyrolyzed bio-
chars produced from agricultural waste ranged from 5.40–7.70 mg g1 P
and the regenerated biochar could re-adsorb up to 5.60 mg g1 at the same
initial P concentration. Although the regeneration of spent waste-based
adsorbents is a promising development, there exists a knowledge gap to
develop a regeneration procedure suitable for use in the field. However,
understanding the principles behind these regeneration methods can enable
more efficient engineering of waste-based materials. For example, Pratt
et al. (2011) found the application of acidic (1 M HCl) and reducing (1 M
Na2S2O4) had the double benefit of recovering P from the active slag filters
as well as potentially liberating and activating new adsorption sites for fur-
ther P removal. Based on this result, the active slag filters can be trans-
ferred into the anaerobic ponds and offered a possible way to regenerate
spent waste-based adsorbents in the large-scale field.
Fifth, engineering application has regarded a popular option to recycle
the spent waste-based adsorbents from both ecological and economic
aspects, industrial waste-based adsorbents in particular. For example, sieved
steel slag is a gravel-like material, making it an excellent cover for construc-
tion. Many states Department of Transportation facilities regularly utilize
steel slag in road construction (Penn & Bowen, 2017). Various kinds of
wastes (i.e., recycled concrete, crushed brick, coal ash) are utilized to pro-
duce cement-based materials and construction products. Furthermore, a
large number of agricultural waste, due to a high amount of cementitious
chemical compounds such as SiO2, CaO, Fe2O3, Al2O3, and MgO, was
applied as a partial cement replacement in many developing counties (Paul
et al., 2019). Roychand et al. (2020) assessed the suitability of granular slag
as a replacement of conventional aggregates in cement concrete after used
for municipal wastewater treatment, and indicated various chemicals con-
tained in municipal wastewater densified the porous slag granules and pro-
vided higher compressive strength compared with conventional and the
raw untreated slag aggregates.
Lastly, energy production is an attractive strategy to dispose of waste-
based adsorbents after used P removal from wastewater, especially for agri-
cultural and forest waste products (Callegari et al., 2020). Depending on
waste properties, the used waste can generate energy through two different
paths: direct combustion or bioenergy production. Direct combustion is the
oldest and easiest way to obtain thermal energy. Many biochars and dried
agricultural wastes are ideal for direct combustion or co-combustion with
other fuel in industrial and domestic activities, ranging from open-fire
stoves or boilers to fluidized bed combustion (Quispe et al., 2017). The
recent approaches for bioenergy production from municipal solid waste

leachate are well explored, as summarized by Gu et al. (2019). There is a
keen interest in biofuels production because it can be used as a supplement
to gasoline or diesel fuel derived from fossil fuels. However, among all
these methods, considering the actual economic and technical level in dif-
ferent regions, direct combustion is still the preferred strategy for bioenergy
recovery. For example, the biosorbents made from biogas residues can be
completely decomposed to fly ash below 550 C, therefore, thermal decom-
position is a technologically feasible method to dispose spent biosorbents
and collect the combustion heat to generate electricity and energy (Pan
et al., 2020).
5. Future perspectives
According to the literature summarized in this review, progress has already
been made toward sustainable phosphorus pollution control by waste-based
adsorbents. While studies have shown that waste-based adsorbents are
effective at removing P from wastewater, there remains a need to improve
their suitability from performance, environmental, and engineering aspects
and turn this research into commercial reality. To this end, the following
recommendations can be made based on this research:
i. Since the waste-based adsorbents can be successfully utilized for phos-
phorus pollution control, most articles focused more on the advantages of
waste-based materials with some limitations rather than their disadvan-
tages. Risk evaluation related to the posttreatment process has, however,
received little concern. For example, these adsorbents may contain toxic
trace elements or organic pollutants that need more detailed analysis for
better recycling after applying them in wastewater treatment.
ii. The specific properties of the waste material and field conditions may
significantly affect the performance of the waste-based adsorbents. Hence,
it is important to make a reference to data representative of both the prop-
erties of the material and real site conditions. This may be achieved by
employing the results of laboratory tests and long-term field monitor-
ing data.
iii. Life cycle assessment (LCA) is a holistic methodology allowing for
the systems and product analysis, which can be applied to waste manage-
ment systems to identify environmental benefits and critical aspects. There
are multiple examples of the application of the LCA method to the pollu-
tion control process in WWTPs (Corominas et al., 2020; Gallego-Schmid &
Tarpani, 2019). Further, LCA studies are needed to evaluate the environ-
mental impacts of phosphorus pollution control by using waste-
based adsorbents.
2046 H. ZHOU ET AL.
iv. The utilization of biochars for phosphorus pollution control can be a

very promising way to dispose of organic waste materials because modified
biochars exhibit excellent P adsorption capacity and can be tailored with
specific properties. Research efforts need to address the heterogeneity of
raw materials to simplify production complexity, reduce the production
cost, and design high-efficiency biochar products. In addition, detailed
manufacturing parameters and the process should be determined for the
development of the biochar industry.
6. Conclusions
In this review, we reported the recent advancement of P pollution control
using waste-based adsorbents and proposed a sustainable paradigm of
waste-based absorbent for P removal utilization as how several strategies
could be incorporated to achieve sustainable P treatment. Based on this
summary, it can be concluded that the “sustainable economy-environment
cycle” should be highlighted when sourcing feedstock for new waste-based
adsorbents. The use of waste-based adsorbents to remove P from aqueous
point sources is a dual valorization of both of these wastes. From a broader
and sustainability perspective, the recapture of P both mitigates its environ-
mental impacts while also conserving a natural resource forecasted to be
increasingly limited in its economically exploitable reserves, and thus, sensi-
tive to market volatility. Apart from resource thriftiness, the capture of P
by adsorbents offers the possibility for its recycling back into the food pro-
duction chain as a P fertilizer in crop production systems. If the anthropo-
genic quadrupling of P circulating in the biosphere has “broken” the global
P cycle (Elser & Bennett, 2011) and is characterizing by a one-way trajec-
tory of P flow up the food production chain (Metson et al., 2016), then,
capturing and re-using P through strategies such as waste-based absorbents
offers a means to circularize and close the otherwise liner and open P cycle.
In many regions of the developing world where waste streams are relatively
less treated, this provides an opportunity to engineer wastewater treatment
plants and other wastewater point sources to recover and valorize P, espe-
cially in co-located regions in the tropics where this nutrient is relatively
limiting to crop production. In developed regions, with highly productive
agriculture, and thus, high P fertilizer needs, the magnitude of P that could
be recoverable from waste streams is appreciable in meeting crop P needs
and can be a way to abate or recoup otherwise high economic costs of P
removal. For example, it has been estimated that in the region of the
north-central US known as the Corn (Maize) Belt, and there is potentially
full self-sufficiency in meeting maize P needs, although economic and agro-
nomic considerations on P recovery may constrain how much of this
potential is realized (Margenot et al., 2019). Addressing context-specificity

of P removal, including locally available waste-based absorbents, is, thus,
needed to increase the circularization of P flows in the anthropogenic
trophic chain.
Overall, this article emphasized the importance of improving P pollution
control treatment sustainability. A sustainable paradigm is proposed based
on the research cases and rational insights: (i) the combination of different
waste-based adsorbents to improve removal performance or adsorb mul-
tiple pollutants; (ii) phosphorus recovery from the spent adsorbents (elu-
tion or direct use as fertilizer); (iii) engineering construction; (iv) energy
production (direct combustion and bioenergy production); and (v) regener-
ation. The waste-based adsorbents have received extensive attention for
their eco-friendly and easily recoverable capability. The apparent advan-
tages of waste-based adsorbents indicate it will have a broad application
space in phosphorus pollution control, especially in developing countries.
Disclosure statement
The authors declare that they have no known competing financial interests or personal
relationships that could have appeared to influence the work reported in this article.
Funding
This work was partially supported by the National Institute of Food and Agriculture, U.S.
Department of Agriculture, Hatch project (No. ILLU-741-337).
ORCID
Hongxu Zhou http://orcid.org/0000-0002-1746-8182
Rabin Bhattarai http://orcid.org/0000-0002-3433-299X
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Phosphorus pollution control using waste-based

KEYWORDS Development and application; phosphorus removal; sustainable management; waste-based

CONTACT Shiyang Li lishiyang1987@gmail.com Key Laboratory of Organic Compound Pollution Control

into the environment (UN-Water, 2019). Even in developed counties, some

in different waste-based adsorbents used to remove P from wastewater. A

2. Phosphorus forms and major phosphorus pollution sources in water

et al., 2015). For non-point sources, agriculture is the main contributor of

3. Waste-based absorbents for phosphorus pollution control

Table 1. P concentrations reported in wastewater from different sources.

3.1. Industrial waste-based adsorbents

to predict the P removal capacity of RM in both low (forest runoff) and

3.2. Agricultural waste-based adsorbents

Through thermal or chemically modifying properties of agricultural waste

eggshell calcination at 900  C for 30 min resulted in 55% and 95% P

3.3. Construction and demolition waste-based adsorbents

3.4. Marine debris-based adsorbents

Table 4. Presentation and evaluation of construction/demolition waste-based adsorbents.

3.5. General consideration

Table 5. Presentation and evaluation of Marine debris-based adsorbents.

Figure 3. The synthesis pathways and P adsorption mechanism of chitosan-calcite adsorbents:

Besides, past studies have evaluated the performance of waste-based adsorb-

3.5.1. Environmental concerns

3.5.2. Economic evaluation

in an economic analysis of regenerating unmodified and modified absorb-

3.5.3. Selection criteria of waste-based adsorbents

4. A sustainable paradigm for waste-based absorbent in P

Figure 4. The sustainable pathway of waste-based adsorbents in phosphorus pollution con-

application – recovery – regeneration – disposal of waste-based adsorbents

potato peel) have an advantage as versatile adsorbents in absorbing inor-

could be applied as a sustainable building block for the preconcentration of

recent approaches for bioenergy production from municipal solid waste

iv. The utilization of biochars for phosphorus pollution control can be a

potential is realized (Margenot et al., 2019). Addressing context-specificity

Sustainable Chemistry & Engineering, 6(3), 3135–3142. https://doi.org/10.1021/acssusche-

phosphate adsorption. Science of the Total Environment, 714, 136839. https://doi.org/10.

furnace slag. Chemical Engineering Journal, 327, 713–724. https://doi.org/10.1016/j.cej.

Romar-Gasalla, A., Rivas-Perez, I. M., Paradelo-N ~ez, R., N

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eggshell calcination at 900 C for 30 min resulted in 55% and 95% P