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Sayeda Ummeh Masrura, Pavani Dissanayake, Yuqing Sun, Yong Sik Ok,
Daniel C. W. Tsang & Eakalak Khan
To cite this article: Sayeda Ummeh Masrura, Pavani Dissanayake, Yuqing Sun, Yong Sik Ok,
Daniel C. W. Tsang & Eakalak Khan (2021) Sustainable use of biochar for resource recovery and
pharmaceutical removal from human urine: A critical review, Critical Reviews in Environmental
Science and Technology, 51:24, 3016-3048, DOI: 10.1080/10643389.2020.1818497
ABSTRACT
Biochar has recently been used
for recovering nutrients from
waste streams including source-
separated human urine. The
increased consumption of phar-
maceuticals has been a subject of
concern as some of the com-
pounds are not completely
metabolized and consequently
present in human urine. As urine contains both nutrients and pharmaceuticals, biochar
applied for nutrient recovery may adsorb pharmaceuticals causing a concern on the intro-
duction of the contaminants to the environment. This review article discusses the sorption
of nutrients as well as pharmaceuticals by biochar. It reveals that biochars with different
properties can be employed to separately attain nitrogen and phosphorus recovery, and
removal of pharmaceuticals from source-separated urine. Production conditions including
pyrolysis temperature and feedstock source are the vital aspects for delivering biochar
properties that are suitable for different groups of chemical entities (nutrients versus phar-
maceuticals). In addition, pharmaceutical adsorption is more favorable at lower solution pH
whereas nutrient recovery is favorable at higher solution pH. If this concept of using separ-
ate biochars is employed, it will minimize the potential exposure of pharmaceuticals to the
environment and humans and in the process the nutrient-rich biochar can be applied to
the agrarian fields to achieve a closed-loop fertility system.
1. Introduction
Municipal wastewater should be considered as a valuable resource because
of its high nutrient contents (phosphorus and nitrogen). For sustainable
nutrient management, urine source separation, a scheme involved in
CONTACT Eakalak Khan eakalak.khan@unlv.edu Department of Civil and Environmental Engineering and
Construction, University of Nevada, Las Vegas, Box 454015, 4505 S. Maryland Parkway, Las Vegas, NV 89154-
4015, USA.
ß 2020 Taylor & Francis Group, LLC
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3017
biochar applied for nutrient recovery from urine can pick up pharmaceuti-
cals. The recovery process reduces the overall pollution (nutrients and
pharmaceuticals) load in the urine stream and eventually natural waters but
utilizing the applied biochar as a soil amendment may lead to unintentional
introduction of the pharmaceuticals to the environment. The overarching
objective of this article is to address this specific scenario. With new
research and developments in biochar-based technologies, there is a possi-
bility to recover nutrients while reducing the risk of introducing pharma-
ceuticals and their metabolites into the environment (Desbiolles et al.,
2018; Li et al., 2020). For this purpose, the selection of specific types of bio-
char based on their sorption properties toward nutrients and pharmaceuti-
cals is essential. If nutrients have more affinities than pharmaceuticals to
biochar, the field application of nutrient-rich biochar can be ensured to
enhance soil productivity with minimal risk of environmental contamin-
ation. Relative affinities of nutrients and pharmaceuticals and their metabo-
lites to biochar are therefore crucial.
Our literature search on Google Scholar, Web of Science, and Elsevier
Science Direct databases was conducted using the keywords “biochar and
nutrients” and “biochar and pharmaceuticals” in the title, abstract, and key-
words. Overall, 116 peer-reviewed journal articles were chosen for this crit-
ical review. The aims of this critical review article are to appraise the
principal mechanisms for separate removal of pharmaceuticals and
nutrients by biochar and to recommend an environmentally sound
approach to recover N and P in urine by biochar for application as a soil
fertilizer with no or limited pharmaceutical contents. In this manner, the
applied biochar, which is rich in N and P, would enhance soil productivity
without contaminating the soil. This issue/approach has not
been discussed.
Several studies evaluated the application of biochar for nutrient recovery
and pharmaceutical removal from wastewater separately (Solanki & Boyer,
2019; Takaya, Fletcher, Singh, Okwuosa, et al., 2016; Trazzi et al., 2016; Xie
et al., 2014); however, none of the studies looked at them together. These
studies described the characteristics and applications of biochar, and inter-
action mechanisms between the contaminants (sorbates) in wastewater and
biochar. Despite significant research and reviews on biochar, there is a
knowledge gap on the application of biochar for separate removal of a mix-
ture of pharmaceuticals and nutrients as found in urine. The idea behind
the recommended approach is to devise two separate biochars with differ-
ent properties and functionalities, one that is selective toward pharma-
ceuticals and the other that mainly adsorbs nutrients. This article
critically evaluates the surface chemistry of biochar and environmental
conditions to elucidate sorption sites and mechanisms for nutrients and
3020 S. U. MASRURA ET AL.
et al. (2016)
Oak sawdust 300 Aqueous LaCl3 50.2 5.8 41.6 0.2 0.9 Wang et al.
400 solution 69.4 4.3 22.4 0.4 2.0 (2015)
(continued)
3023
Table 1. Continued.
3024
Phosphorus Sesame straw 300 Aqueous ZnCl2 58.1 5.2 33.4 2.4 Park et al.
400 solution 61.7 4.7 31.2 2.5 (2015)
500 64.2 4.2 30.2 2.7
600 72.6 2.1 21.7 2.9
Miscanthus x giganteus 700 Aqueous 7.0 90.4 1.7 7.5 0.5 14.9 Trazzi et al.
Sugarcane bagasse 700 solution (2016)
86.5 1.9 11.1 0.5 12.5
Wheat straw 500–550 Aqueous 3.0–11.0 86.9 2.6 8.9 1.3 31.8 Dugdug et al.
Hardwood 500–550 solution 89.2 2.7 7.9 0.2 35.8 (2018)
Willow wood 500–560 86.7 2.2 10.3 0.8 37.7
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3025
(>50 nm) (Li et al., 2017). Biochars produced from different types of wood
and bamboo have meso/macroporous structures while those produced from
husks exhibit microporous structures (Joseph et al., 2007). The removal of
volatile materials from biochar at high pyrolysis temperatures results in the
development of micropores (Ahmad et al., 2012) and thereby improved
adsorption capacity (Sun et al., 2014). Generally, biochar produced at lower
temperatures has a higher yield than the biochar produced at higher tem-
peratures as organic matter decomposition rate increases with temperature
(Sun et al., 2014). Biochar pyrolyzed at high temperatures results in more
specific surface area and aromaticity (Ahmad et al., 2012) but less H and O
components (Gai et al., 2014). For example, biochar pyrolyzed at 600 C
showed 30 times greater surface areas than the biochar prepared at 450 C
(Sun et al., 2014). Larger surface areas indicate more porous structures
within biochar to adsorb chemical compounds.
Takaya, Fletcher, Singh, Anyikude, et al. (2016) inspected the effect of
feedstocks on the physicochemical properties of biochar such as surface
functionality, pH, CEC, and mineral contents. Manure biochar has higher
ash contents because of the presence of minerals (calcite and quartz) facili-
tating phosphate adsorption (Cao & Harris, 2010). Recent studies explored
different engineering approaches to alter biochar surface by metal oxides to
increase the adsorption capacity for phosphate from human urine (Park
et al., 2015; Xu et al., 2019; Zheng et al., 2018). Among different activation
agents, biochar surface modified with MgO resulted in better adsorption
capacity for phosphate (Xu et al., 2018, 2019; Zheng et al., 2018). Previous
analyses have reported that phosphate adsorption capacity of biochar
increases with production temperature up to 500 C (Takaya, Fletcher,
Singh, Anyikude, et al., 2016; Wang et al., 2015) as pores in the biochar are
blocked with further increase in the pyrolysis temperature (Jung et al.,
2016). However, a different study reported that phosphate adsorption cap-
acity of biochar was hardly affected by pyrolysis temperature (Lou et al.,
2016). Phosphorus sorption capacity of biochar is controlled by the initial
phosphate concentration more than the type of feedstock and pyrolysis
conditions. The reactive adsorption sites on biochar surface filled better at
higher concentration gradients (Dugdug et al., 2018; Takaya, Fletcher,
Singh, Anyikude, et al., 2016; Trazzi et al., 2016).
Biochar usually carries negative surface charge, which boosts the ability
to adsorb and hold cations (NH4þ) (Gai et al., 2014; Zheng et al., 2018).
Some studies reported that NH4þ adsorption was not influenced by biochar
surface area (Cai et al., 2016; Gai et al., 2014; Takaya, Fletcher, Singh,
Anyikude, et al., 2016). Ammonium adsorption by biochar is characterized
by chemical bonding and electrostatic interaction of ammonium with the
surface functional group (Yang et al., 2018). Biochars pyrolyzed at lower
3026 S. U. MASRURA ET AL.
3.2. Recovery of N
Urea, a major nitrogen component in human urine, rapidly undergoes
decomposition during storage to ammonia. As a result, urea recovery by
biochar has not been widely studied. For low urea concentrations in human
urine (<4000 mg L1), biochar prepared at low temperature manifested
greater urea adsorption capacity than that prepared at high temperature
because of more C ¼ O and/or C-H on the surface that could act as poten-
tial sites for nutrient interaction (Gai et al., 2014; Zhang, Li, et al., 2015).
Biochar prepared at high pyrolysis temperatures had low polarity result-
ing in less NH4þ adsorption capacity (Gai et al., 2014). Oxygen-containing
functional groups such as C ¼ O, COOH, and COC contributed sub-
stantially to NH4þ adsorption because of hydrogen bonds and electrostatic
interaction between NH4þ and biochar (Cai et al., 2016). The sorption cap-
acity of NH4þ-N decreased after washing biochar with deionized water and
acid as the process washed off ash content and some inorganic fractions
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3027
3.3. Recovery of P
Surface functionality of biochar surface may not influence phosphate adsorp-
tion due to negatively charged surface (Takaya, Fletcher, Singh, Anyikude,
et al., 2016; Yao et al., 2011). The adsorption of P on biochar was affected
by the concentration of phosphate in solution, pyrolysis temperature, and
adsorption time. Higher phosphate concentrations in the solution, increased
pyrolysis temperature (up to 500 C), and longer residence time resulted in
the highest adsorption capacity (Takaya, Fletcher, Singh, Anyikude, et al.,
2016; Trazzi et al., 2016). The main forms of phosphate in urine are
HPO42 and H2PO4 at a pH range of 3–7 (Trazzi et al., 2016; Yang et al.,
2019). At pH above 7, OH strongly competes with PO43 in the solution
for active sites, leading toward lower phosphate adsorption capacity (Dugdug
et al., 2018; Jung et al., 2015; Trazzi et al., 2016; Yang et al., 2019).
Chen et al. (2011) studied the adsorption of phosphate by magnetic and
nonmagnetic biochars. The results displayed that the sorption efficacy of mag-
netic biochar was considerably greater than the companion biochar pyrolyzed
at a similar temperature, indicating the positive impact of the presence of iron
oxides for better adsorption of phosphate (Chen et al., 2011; Peng et al.,
2019). Dolomite-modified biochar formed lamellar structures via decompos-
ition of dolomite into magnesium and calcium oxides to offer binding sites
for phosphate at lower solution pH (Li et al., 2019). Biochar activated with
ZnCl2 improved phosphorus adsorption capacity by flaring the pores and pro-
ducing more positive sites on biochar surface (Park et al., 2015).
Diclofenac Pine chips 300 Aqueous solution 3.5 Jung et al. (2013)
Bamboo >315 Synthetic and 6.0 and 9.0 Solanki and
Softwood pine 550 real urine Boyer (2017)
Coconut shell 400–500
Northern 400–500
hardwood
Ibuprofen Pine chips 300 Aqueous solution 3.5 Jung et al. (2013)
Bamboo >315 Synthetic and 6.0 and 9.0 Solanki and Boyer (2017)
Softwood pine 550 real urine
Coconut shell 400–500
Northern 400–500
hardwood
Naproxen Bamboo >315 Synthetic and 6.0 and 9.0 Solanki and Boyer (2017)
Softwood pine 550 real urine
Coconut shell 400–500
Northern 400–500
hardwood
Bamboo >315 Synthetic and Solanki and Boyer (2019)
Softwood 550 real urine
Sulfamethoxazole Pine 650 Aqueous solution 4.0–9.0 FeCl2 Reguyal et al. (2017)
sawdust
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY
biochar
Pine chips 300 Aqueous solution 3.5 Jung et al. (2013)
Bamboo 550 Aqueous solution 3.0–9.0 CuZnFe2O4 Heo et al. (2019)
Giant reed 300–600 Aqueous solution 1.0–6.0 Zheng et al. (2013)
3029
Tea waste 300 and 700 Water 3.0–9.0 Rajapaksha, Vithanage, Zhang, et al. (2014)
(continued)
Table 2. Continued.
3030
Pyrolysis
Pharmaceuticals Feedstock temperature ( C) Adsorbate media Solution pH Chemical agent References
Sulfamethazine Wheat and 30 and 600 Aqueous solution 1.5–10.2 Jia et al. (2018)
maize straw
Burcucumber 700 Aqueous solution 3.0–9.0 Rajapaksha et al. (2015)
plant
Tea waste
S. U. MASRURA ET AL.
Tetracycline Rice husk 450 Wastewater 2.0 CH3OH Jing et al. (2014)
Cow manure 300–700 Aqueous solution 3–10 Zhang et al. (2019)
Rice straw 700 Aqueous solution 5.0–9.0 H3PO4 Chen et al. (2018)
Swine manure
Bamboo 700 Deionized water 5.0–7.0 SiO2 Zhao et al. (2019)
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3031
et al., 2014; Rajapaksha, Vithanage, Zhang, et al., 2014; Zheng et al., 2013).
For example, SMX being a strong p-acceptor due to N-heteroaromatic
rings and amino functional groups interacts with high temperature biochar
which is a p-donor due to less carboxyl functional groups and high content
of graphitic carbon (Zheng et al., 2013). Similar p-p interactions were
observed during biochar adsorption of TC (Peiris et al., 2017) and
naproxen (Tomul et al., 2020). A study on microalgae derived biochar
showed that the presence of Ca3(PO4)2, CaCO3, and CaNaPO4 may affect
TC adsorption through the metal complexation process (Choi et al., 2020).
As manure-based biochar contains higher ash content and surface oxygen
content, it should be less effective for the adsorption of pharmaceuticals.
Jung et al. (2013) compared the adsorption capacity of four pharmaceuti-
cals (carbamazepine, SMX, ibuprofen, diclofenac) on biochar generated
under oxygen-free (N-biochar) and oxygenated (O-biochar) conditions. N-
biochar contained better polarity moieties content but less aromaticity than
that of O-biochar. While high aromaticity contributed to adsorption,
increased pore volume and surface area of N-biochar led to greater sorp-
tion for pharmaceuticals.
The adsorption capacity of pharmaceuticals can be enhanced by chemical
activation of biochar surface as a result of enhanced surface areas, pore
structures, and interactions with specific surface functional groups. For
example, a surface modification with acid or alkaline substances increased
the availability of oxygen containing functional groups and resulted in
42.92% increase in amoxicillin adsorption (Li et al., 2017). Thermal treat-
ment by using air/nitrogen mixture promoted the mesoporosity on the sur-
face of biochar leading to improved TC adsorption by 5.5–9.2 folds (Zhu et
al., 2018). Steam activated biochar removed 98% more SMZ than non-acti-
vated biochar owing to improved porous structure with larger pore diame-
ters (Rajapaksha et al., 2016).
Solanki & Boyer, 2019; Zhang et al., 2019). On the contrary, nutrient
adsorption tends to be more prevalent at higher solution pH. A potential
process for SMZ sorption on biochars at low pH can be described by p-p
EDA interactions between the electron-rich graphene surfaces and proto-
nated amino groups on the aromatic ring (Rajapaksha, Vithanage, Zhang,
et al., 2014; Teixido et al., 2011). Electrostatic interactions and charge dif-
ferential between biochar and pharmaceuticals stimulated the removal of
negatively charged pharmaceuticals, for example, naproxen, ibuprofen, and
diclofenac (Solanki & Boyer, 2017).
The adsorption efficiency of pharmaceuticals decreases with increasing
adsorbate concentration. In contrast, elevating biochar dose will bring
about a better adsorption efficiency, but the treatment cost will increase
(Teixido et al., 2011). The adsorption capacity of biochar for pharmaceuti-
cals enhanced with adsorbent dosage due to a greater number of adsorption
sites and larger surface areas (Shang et al., 2016; Solanki & Boyer, 2017;
Zhang et al., 2019). The contact time between biochar and pharmaceuticals
needs to be chosen in a way that maximum removal can be achieved at
minimum contact time. The longer contact time provided better adsorption
capacity (Solanki & Boyer, 2019) and maximum uptake occurred in the
first 24 h (Teixido et al., 2011). For instance, biochar prepared from soft-
wood delivered the highest sorption capacity for naproxen and paracetamol
with the longest contact time studied (5 days) (Solanki & Boyer, 2019).
Adsorption of the antibiotic SMZ on biochar is a function of adsorbate
pH, competing organic compounds, and inorganic background ions
(Teixido et al., 2011). In general, the maximum sorption efficiency of anti-
biotics was achieved at lower pH values. The p-p EDA interaction con-
trolled the sorption capacity at low pH as SMZ and biochar both were
positively charged. Biochar surface became negatively charged at lower pH,
and the adsorption capacity of SMZ improved due to cation-p bonding
and electrostatic attractive force (Jia et al., 2018).
At pH >6.0, negative charge-assisted hydrogen bond (CAHB) dominated
the adsorption as the SMX and biochar both had negative surface charge
(Li et al., 2014). However, Shang et al.(J. G. Shang et al., 2016) showed that
biochars pyrolyzed at 800 C had maximum adsorption of ciprofloxacin at
pH 7, while the adsorption capacity reduced with the change of pH from 7
to 10. The removal of ciprofloxacin was attributed to the formation of
hydrogen bonding and extents of ionization of ciprofloxacin at different
pH (Li et al., 2014). In a different study, the adsorption of SMX on mag-
netic pine sawdust biochars (MPSB) was affected negatively with the
increase in pH. At higher pH, the negative species present in SMX was
more dominant and had less affinity to MPSB (Reguyal et al., 2017).
Additionally, the presence of humic acid could create obstruction for SMZ
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3033
Figure 1. Effect of pH on adsorption of ammonium using corn cob biochar (Vu et al., 2017),
phosphate using wheat straw biochar (Dugdug et al., 2018) and sulfamethazine removal using
bur cucumber biochar (Rajapaksha et al., 2016).
Figure 2. Effect of pyrolysis temperature on adsorption of ammonium using Pine sawdust bio-
char (Yang et al., 2018), phosphate using Pine sawdust biochar (Lou et al., 2016) and tetracyc-
line removal using Cow manure biochar (Zhang et al., 2019).
Figure 3. Schematic diagram of the process for recovery of nutrients and removal of
pharmaceuticals.
along with nutrients at the first setting, and may be emitted to the environ-
ment during the application of nutrient-rich biochar to the field. Figure 3
displays the schematic representation of this process.
If the filter setting is placed in a way that biochar adsorbs pharmaceuti-
cals first and then another biochar is employed for nutrient recovery, the
problem of environmental release would be substantially less. However, pH
would need to be adjusted twice; first below 5 for removal of pharmaceuti-
cals and then above 7 for nutrient recovery. In that case, biochar removes
most of the pharmaceuticals in the first filter and only low levels of them
remain in the urine stream. The second filter, designed for adsorption of
nutrients, may adsorb the remaining pharmaceuticals along with nutrients,
thereby the risk of soil contamination would be less.
These concepts of using two separate biochars in sequence if applied to source-
separated urine will yield nutrient-rich biochar that will not cause the environ-
mental concern of pharmaceuticals release. In addition, the contaminants (phar-
maceuticals and metabolites) in the urine stream get removed separately at the
source before they are diluted into the wastewater stream. These outcomes are the
best among those delivered by all the different schemes discussed above.
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3037
6. Conclusions
Biochar, a promising and environmentally friendly adsorptive material, can
serve as recovery and treatment media for nutrients and pharmaceuticals,
respectively, from source-separated urine. Application of nutrient-rich bio-
char to low fertility soil can contribute to the habilitation of soil and crop
productivity. This review highlights that the types of feedstock, pyrolysis
conditions, biochar properties, and pH values are the principal factors
influencing biochar adsorption capacities of nutrients and pharmaceuticals.
Using biochar for recovery and delivery of nutrients from urine could
transfer pharmaceuticals to agricultural fields. As emphasized in this
review, separate extraction of nutrients and pharmaceuticals using two dif-
ferent biochars can be placed in a series to eliminate the problem of intro-
ducing pharmaceuticals into the environment. For the proposed in-series
extraction process, low temperature (from 300 to 500 C) biochar is
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 3039
ORCID
Yong Sik Ok http://orcid.org/0000-0003-3401-0912
Daniel C. W. Tsang http://orcid.org/0000-0002-6850-733X
Eakalak Khan http://orcid.org/0000-0002-6729-2170
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