Comparison of Pyrolysis Process Various Fractions PDF

Ecotoxicology and Environmental Safety 208 (2021) 111756
Contents lists available at ScienceDirect
Ecotoxicology and Environmental Safety

journal homepage: www.elsevier.com/locate/ecoenv
Review
Comparison of pyrolysis process, various fractions and potential soil

applications between sewage sludge-based biochars and
lignocellulose-based biochars
Jia Xing a, Guoren Xu a, b, *, Guibai Li a
a
School of Environment, Harbin Institute of Technology, Harbin 150090, China
b
College of Resources and Environment, University of Chinese Academy of Sciences (UCAS), Beijing 100049, China
A R T I C L E I N F O A B S T R A C T
Editor by Professor Bing Yan To deeply assess the feasibility of sewage sludge-based biochars for use in soil applications, this review compared
sewage sludge-based biochars (SSBBs) with lignocellulose-based biochars (LCBBs) in terms of their pyrolysis
Keywords: processes, various fractions and potential soil applications. Based on the reviewed literature, significant differ
Organic carbon ences between the components of SSBB and LCBB result in different pyrolysis behavior. In terms of the fractions
Mineral component
of biochars, obvious differences were confirmed to exist in the carbon content, surface functional groups, types of
Trace element
ash fractions and contents of potential toxic elements (PTEs). However, a clear influence of the feedstock on
Polycyclic aromatic hydrocarbons
Soil remediation labile carbon and polycyclic aromatic hydrocarbons (PAHs) was not observed in the current research. These
differences determined subsequent discrepancies in the soil application potential and corresponding mecha
nisms. The major challenges facing biochar application in soils and corresponding recommendations for future
research were also addressed. LCBBs promote carbon sequestration, heavy metal retention and organic matter
immobilization. The application of SSBBs is a promising approach to improve soil phosphorus fertility, immo
bilize heavy metals and provide available carbon sources for soil microbes to stimulate microbial biomass. The
present review provides guidance information for selecting appropriate types of biochars to address targeted soil
issues.
1. Introduction bring about much more uncertainty in the feasibility of SSBB for use in
soil applications.
Rapid population growth and high urban development have Lignocellulosic biomass is one of the most traditional feedstocks in
increased the production of sewage sludge (Collivignarelli et al., 2019). use for pyrolysis, with its major sources being from wood as well as
Therefore, there is an urgent need for proper disposal of sewage sludge herbaceous and agricultural biomass (HAAB). The feedstock is mainly
around the world. Recently, pyrolysis has arisen as a novel option for composed of aromatic polymers (lignin) and carbohydrate polymers
sewage sludge management. High temperatures can effectively kill (cellulose and hemicellulose) (Li and Jiang, 2017), and pyrolysis con
pathogenic organisms and minimize sewage sludge volume. During verses lignocellulosic biomass into high-quality fuels, chemical products
pyrolysis process, sludge gradually undergoes organic matter degrada and lignocellulose-based biochars (LCBBs). Due to the unique porous
tion and minerals oxidation (Jin et al., 2016), finally producing sewage structure and surface chemistry, LCBBs have been widely used as
sludge-based biochars (SSBBs). Given the abundant carbon and plant low-cost and efficient amendments in use for soil remediation. Mean
nutrients, SSBB has aroused wide interests to be used as a soil amend while, the application of LCBBs in soils can provide multiple benefits.
ment. However, high levels of heteroatoms and inherent heavy metals For example, application of LCBB derived from rice straw was found to
Abbreviations: SSBBs, Sewage sludge-based biochars; LCBBs, Lignocellulose-based biochars; HAAB, Herbaceous and agricultural biomass; XRD, X-ray diffraction;
DOC, Dissolved organic carbon; DOM, Dissolved organic matter; PAHs, Polycyclic aromatic hydrocarbons; PTEs, potential toxic elements; IBI, International biochar
initiative; EBC, European biochar certificate; HOCs, Hydrophobic organic compounds; NMR, Nuclear magnetic resonance; GWP, Global warming potential; MPSP,
minimum product selling prices; NPV, net present value; TTEC, Total toxic equivalent concentration; EPFRs, environmentally persistent free radicals.
* Corresponding author at: School of environment, Harbin Institute of Technology, Harbin 150090, China.
E-mail address: xgr@hit.edu.cn (G. Xu).
https://doi.org/10.1016/j.ecoenv.2020.111756
Received 26 August 2020; Received in revised form 9 November 2020; Accepted 30 November 2020
Available online 8 December 2020
0147-6513/© 2020 The Author(s). Published by Elsevier Inc. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
J. Xing et al. Ecotoxicology and Environmental Safety 208 (2021) 111756
increase up to 209.87% soil organic matter and reduced the contents of pyrolysis process, and have also been widely concerned.
available Cu and Cd by 5.8–45.32% and 15.69–17.65% in acidic soils, Currently, a variety of biochars from different feedstock sources have
respectively (Chen et al., 2020). LCBB also achieved long-term carbon been reviewed extensively. However, few reviews focus on the pyrolysis
sequestration in paddy soils, which was revealed by slight 1.16% processes, properties and applications of SSBB in soils, and differences
organic carbon losses in four years (Bi et al., 2020). between SSBBs and LCBBs are seldom emphasized. This knowledge is
Biochar is a heterogeneous mixture with different fractions, essential to accurately define and classify biochars derived from sewage
including carbon pool, labile carbon pool, ash fraction, and even inor sludge and lignocellulosic biomass. Additionally, the clear distinction
ganic/organic contaminants. The contents and properties of different between SSBBs and LCBBs benefits to explore the linkage between py
fractions are mainly determined by the biomass feedstock and pyrolysis rolysis processes, properties and applications as well as their sources of
temperature. Sewage sludge and lignocellulosic biomass respond het feedstock biomass, which can provide guidelines for selecting appro
erogeneously to particular pyrolysis temperature owing to variations of priate biochars to address targeted soil issues.
organic composition and inorganic mineral components contents, The present review summarizes the differences between SSBBs and
therefore, resulting in the variations of different fractions contents and LCBBs in terms of their pyrolysis processes and multiple fractions,
distinctive physicochemical properties between SSBBs and LCBBs (Wei including: (i) the stable carbon pool; (ii) the labile carbon pool; (iii) the
et al., 2019). Within the pyrolysis temperature range, the abundant ash fraction, (iv) the contaminants. The soil application potential of
cellulose, hemicellulose and lignin in lignocellulosic biomass are grad SSBBs is also compared with that of LCBBs. The differences between
ually degraded at different rates to form compact carbon skeletons for SSBBs and LCBBs in pore structures are also reviewed in the supple
LCBBs. A large quantity of ash fractions in sewage sludge can be mentary material. This review seeks to offer a rational assessment of
enriched with elevated pyrolysis temperatures and participate in sludge current knowledge and what needs to be done in future research, with
pyrolysis to affect structural characteristics of SSBB carbon pool (Wei implications for the resource utilization of biochars in soils.
et al., 2016; Li et al., 2018b).
As various fractions in biochars simultaneously participate in soil 2. Pyrolysis process of biomass
applications (Fig. 1), variations of fractions contents and distinctive
physicochemical properties between SSBBs and LCBBs consequently 2.1. Pyrolysis process of lignin, cellulose and hemicellulose
cause different application potential and effects. Oxygen-containing
functional groups are known to increase soil cation exchange capacity Cellulose has a simple composition and structure and is composed of
and contribute to the retention of heavy metals in weathered acidic soil glucose linked by β-1,4-glycosidic bonds (Liang et al., 2018). In the
(Uchimiya et al., 2011a). Aromatic structures can adsorb organic com initial pyrolysis process, the β-1,4-glycosidic bonds between glucose
pounds via π-π interactions (Bielska et al., 2017), and determine the units begin to break, resulting in a decreased polymerization degree of
carbon sequestration ability of the biochar (McBeath et al., 2015). cellulose (Liang et al., 2018) and the generation of increasing numbers
Mineral compounds released from biochars contribute to the neutrali of monomer units (Fig. 2(a)). Subsequently, monomer units undergo
zation of acidic soils (Dai et al., 2017), immobilization of heavy metals intramolecular rearrangement to form levoglucosan (Shen and Gu,
via surface precipitation and cation exchange (Uchimiya et al., 2011b; 2009). Levoglucosan is assumed to be the key intermediate determining
Fang et al., 2016), and act as an additional fertilizer to improve soil the formation of anhydro-monosaccharides through isomerization and
fertility (Ding et al., 2016). Contaminants have also been detected in dehydration reactions, which eventually form solid biochars via poly
biochars, originating from waste biomass or forming along with the merization, dehydration and fragmentation (Kawamoto et al., 2003).
Fig. 1. Proposed roles of carbon pool, liable carbon pool and ash fractions in soils applications and potential ways for contaminant to impact soils.
2
Fig. 2. Pyrolysis process of cellulose (a), hemicellulose (b) and lignin (c).
The amorphous structures of hemicellulose reduce the possibility of dehydration reactions (Yang et al., 2019b). These reactions lead to the
cross-linking reactions, therefore, intramolecular dehydration reaction formation of anhydrosugars, such as 1,4-anhydro-D-xylopyranose and 1,
is responsible for most of the weight loss in the initial pyrolysis process 2:3,4-dianhydrosugars (Yang et al., 2019b) (Fig. 2(b)). These interme
(Yang et al., 2019b). Thereafter, the glycosidic linkages between diate products further undergo dehydration, decarboxylation, aromati
monomer units become very active and begin to cleave via a series of zation and intramolecular condensation to form solid residues,
concerted reactions, including enol-keto tautomerization and condensable bio-oil and syngas (Liu et al., 2015).
3
Lignin is a complex polymer of phenylpropane units comprised of 3. Carbon pool

different aromatic ring substitution patterns, all of which are randomly
linked together through various ether linkages and condensed bonds 3.1. Stable carbon pool
(Wang et al., 2015a; Kawamoto, 2017). In the initial pyrolysis stage, the
weak internal linkages between phenylpropane units, such as ether Stable carbon pool, including aliphatic carbon, aromatic carbon and
linkages, are rapidly ruptured via hemolytic and heterolytic mechanisms functional groups, is the essential component of biochars and determine
(Liu et al., 2016; Kawamoto, 2017). Then the condensed bonds become biochar functionality as soil amendments. The content and properties of
active and begin to break, promoting the production of lignin mono stable carbon are highly influenced by feedstock and pyrolysis temper
mers. The pyrolysis products can undergo re-polymerization reactions atures. As shown in Table S1, the total carbon content of LCBBs is in the
via the condensed linkages and are finally converted to solid char range of 38.7-90.9%, and increase as the pyrolysis temperatures in
products. creases. The high contents of cellulose fractions in feedstock facilitate to
prepare biochars with lower C contents (Zhao et al., 2014), whereas a
2.2. Pyrolysis process of sewage sludge greater proportion of lignin leads to the production of biochars with
higher C contents. Therefore, HAAB-based biochars generally contain
Protein in sewage sludge has different pyrolysis pathways from those lower C contents than wood-based biochars. The increase in the C
of plant residues. Deamination and dehydrogenation can result in the content of LCBB with increasing pyrolysis temperature is probably due
decomposition of protein, accompanied with the disappearance of to the increasing degree of carbonization (Wei et al., 2019), indicating
–CHON- in SSBBs and the emission of gaseous N compounds, such as the transformation from aliphatic carbon to aromatic carbon as tem
NH3 and HCN (Zhang et al., 2011; Zhang et al., 2013). Meanwhile, peratures rise. This trend can be confirmed by the changes of functional
heterocyclic-N can be generated through the thermal cracking or poly groups on the surfaces of LCBBs. A large proportion of lignocellulose in
merization of N-containing compounds and be structurally integrated feedstocks results in retention of many oxygen-containing functional
into the carbon matrix (Fig. 3). Tian et al. (2013) found that the during groups on the surface of LCBB, including aliphatic carboxyl, hydroxyl
the sludge pyrolysis process, heterocyclic-N increased from 4.6% to 14% and ether groups (Fig. S1) (Chen et al., 2012; Zhao et al., 2018). These
as the pyrolysis temperatures increased from 500 to 800 ◦ C, the authors functional groups gradually decrease in their intensities with increasing
also detected the appearance of quaternary nitrogen and nitrile nitrogen pyrolysis temperatures. In contrast, aromatic skeletal vibration and ar
in biochars during the sludge pyrolysis process. omatic C-H deformation increase at high pyrolysis temperatures. O/C
Inorganic mineral components also participate in sludge pyrolysis ratio and H/C ratio indicate the polarity and degree of aromaticity of
process via several pathways (Magdziarz and Werle, 2014) and cannot biochars, which are critical properties for biochars to evaluate their
be neglected. The main pathways include (i) thermal degradation of carbon structures. In general, high-temperature biochars possess a small
mineral components, (ii) catalytic effect of mineral oxides on sludge number of oxygen-containing functional groups and a large amount of
degradation, (iii) interactions between mineral components and aromatic carbon, thereby featured with lower O/C ratio and H/C ratio,
nitrogen-containing compounds. Calcite (CaCO3) and dolomite (CaMg indicating lower polarity and higher aromaticity. Wood-based biochars
(CO3)2), commonly present in sewage sludge, can be decomposed to CaO tend to have a higher degree of aromaticity and lower H/C ratios
at high temperatures (Zhang et al., 2015). CaO promotes the evolution (McBeath et al., 2014), which might be related to the particular aromatic
and diffusion of volatile matters and decreases activation energies for structures of lignin in feedstock, as well as lower contents of ash, ni
sewage sludge pyrolysis (Guo et al., 2019) The catalytic effect is varied trogen and volatile matter. HAAB-based biochars show higher polarity
with pyrolysis temperatures and sewage sludge composition. Besides, and greater O/C ratios due to their rich O-containing functional groups.
the addition of chemical conditioner to sewage sludge for dewatering, Particular feedstock component in sewage sludge gives rise to the
such as CaO and ferric salt, was reported to interact with sewage sludge unique characteristics of stable carbon of SSBBs, which can be confirmed
protein and affect N conversion and gaseous N emissions in sewage on the surface functional groups of SSBBs. In addition to common
sludge (Zhang et al., 2014; Wei et al., 2016). CaO can directly react with organic functional groups, N-O groups and mineral compounds such as
nitrogen to promote the N retention in the solid residues. It also can kaolinite and quartz can be observed on the surface of SSBB (Fig. S1) (Li
promote the formation of nitriles, which are the main sources of HCN. et al., 2018b), which originate from proteins and mineral components in
Moreover, HCN and H2O can be catalyzed by CaO to produce NH3 and sewage sludge. The high levels of inherent mineral content in sewage
CO. Iron compounds facilitate ring-opening of heterocyclic-N with the sludge result in most SSBBs containing lower total contents of carbon
release of HCN. These interactions result in the insertion of mineral el than LCBBs. Especially for chemical SSBBs, the addition of chemical
ements into carbon matrix and complex sludge pyrolysis process. flocculant further lowers the content of carbon. Additionally, the high
inherent mineral content in sewage sludge also influence stable carbon
Fig. 3. Reactions of amide and mineral substances during pyrolysis of sewage sludge.
4
pool in other ways, leading to the different characteristics of stable et al., 2017b), which represents only a small proportion of the organic
carbon of SSBBs from those of LCBBs. Mineral components have higher residue in biochar but is significant in terrestrial biogeochemical process
thermostability than organic carbon and hence less weight loss. Mineral (Jamieson et al., 2014; Hartley et al., 2016; Igalavithana et al., 2017).
components enrichment outweighs the degree of carbonization (Li et al., The dissolved organic carbon (DOC) content is commonly used to
2018b), leading to the decreased carbon contents of SSBB with represent the content of the dissolved organic matter (DOM) (Maizel
increasing pyrolysis temperatures. High contents of quartz, carbonate, et al., 2017), which is affected by the pyrolysis temperature, biomass
kaolinite and metakaolin can also result in an increase in O and H feedstock and extraction method (Tang et al., 2016; Li et al., 2017; Wei
contents (De la Rosa et al., 2014; Li et al., 2018b), leading to higher H/C et al., 2019). An obvious difference in DOC content can be found among
ratios. Moreover, mineral components may restrict the diffusion of heat the LCBBs in Table S2. Wood-derived biochars have lower contents of
and the release of degraded volatiles during the charring process, which DOC than HAAB-based biochars (Gaskin et al., 2008; Wei et al., 2019).
further hinder the formation of aromatic carbon and contribute to a DOM is indicated to originate from the recondensation of pyrolytic
greater H/C ratio (Xu and Chen, 2013). However, the mineral phase may volatile matter on the surface and pores of biochars (Smith et al., 2016).
also obscure the presence of aromatic structures in carbon fractions (Li The recalcitrant nature of lignin in wood resists thermal decomposition
et al., 2018b), which may impact the accurate assessment of aromaticity. from stable organic carbon to volatile matter, a reason leading to the
For instance, Li et al. (2018b) reported that X-ray diffraction (XRD) did lower contents of DOC. Variations in DOC contents with respect to py
not reveal any obvious turbostratic structure of the carbon fraction in rolysis temperature is also considered, which is the result of degradation
SSBB, while the characteristic peaks of the turbostratic structure and and polymerization. As pyrolysis progresses, organic compounds in
aromatic layer were revealed after acid washing (Fig. 4). biomass undergo continual decomposition and transformation to pro
duce small molecular DOM and CO2, CH4, H2, and H2O (Wei et al.,
2019), characterized by decreased DOC content. Secondary reactions
3.2. Labile carbon pool induced by higher temperature, such as decarboxylation, demethylation
and depolymerization, may lead to further reductions in DOC content
The labile carbon pool of biochar is also known as dissolved biochar (Lin et al., 2012). Polymerization reactions utilize unsaturated hydro
or pyrogenic dissolved organic carbon (Uchimiya et al., 2015; Chen carbons in DOM to promote the production of higher proportions of
condensed aromatics. Thus, in low-temperature LCBB, DOM is featured
with larger DOC content, higher proportions of unsaturated hydrocar
bons and greater H/C ratio. On the other hand, in high-temperature
LCBB, DOM contains smaller amounts of DOC, higher proportions of
condensed aromatics and possesses minor H/C ratio (Chen et al., 2017b;
Kim et al., 2020).
The content of DOC in SSBB is comparable to HAAB-based biochars,
which was found to decrease with increasing pyrolysis temperatures.
Wei et al. (2019) also reported that the total content of DOC in SSBB
decreased much faster than that in LCBB. These results indicated that the
nature of sewage sludge is still liable to thermal degradation although a
large quantity of mineral compounds in sewage sludge. However,
limited information has been obtained on the characteristics of DOM
derived from SSBB. Therefore, it is difficult to compare the character
istics of DOM from SSBB and LCBB. Some studies investigated the
structural changes and composition of DOM derived from biochars as a
function of temperatures. It was found that both SSBB and LCBB con
tained fulvic and humic acid-like compounds (Uchimiya et al., 2013;
Zhang et al., 2015). The distribution of components in DOM varied with
pyrolysis temperatures (Uchimiya et al., 2013; Zhang et al., 2015),
which might be related to the feedstock composition and the trans
formation of intermediate products. Tang et al. (2016) reported that
DOM derived from SSBB was obviously higher in the aromaticity and
molecular weight than that of LCBBs. However, a contrary result was
reported by Wei et al. (2019). The inconsistent results might be due to
the differences in the feedstock, pyrolysis equipment, pyrolysis tem
peratures and extraction methods. Till now, the relationship between
feedstock and DOM characteristics is not established definitively and
require further investigation.
4. Ash fractions
LCBB contains a lower ash fraction in the range of 1.1–37.9%

(Table 1), of which composition and content vary depending on type of
biomass and pyrolysis temperature. Wood-based biochars generally
contain a very low ash content that rarely exceed 10% by weight, and
HAAB-based biochars have a slight higher content of ash fractions due to
rich alkali and alkaline earth metals. Potassium (K) is mainly dominant
in the inorganic fraction of LCBBs. K in plants residues exists in the form
Fig. 4. XRD patterns of sewage sludge (SS) and sewage sludge-based biochars of organic K and inorganic salts, which can combine with the active
(a) before (SS200-700) and (b) after acid washing (HSS200-700). functional groups or intercalates in char layers to form insoluble char K
(Reproduced from Li et al. (2018b), with permission from the publisher). (Zhao et al., 2015; Chen et al., 2017a). Organic K and char K can also
5
Table 1
Comparison of ash fractions between sewage sludge-based biochars and lignocellulose-based biochars.
Feedstock Temperature Ash content P (%) K (%) Ca (%) Mg (%) Reference
(◦ C) (%)
Sludge Dewatered sewage 300 37.42 10.43 2.25 5.33 1.35 Zhang et al. (2015)
sludge
Dewatered sewage 400 49.17 11.56 2.48 5.59 1.42 Zhang et al. (2015)
sludge
sludge
sludge
sludge
sludge
sludge
Residual sewage sludge 680 12.61 ND ND ND ND Srinivasan et al. (2015)
Digested sewage sludge 300 65.8 38.8 7.47 20.6 7.47 Yuan et al. (2015)
Digested sewage sludge 600 83.8 45.1 13.3 24 13.3 Yuan et al. (2015)
Chemical sewage sludge 300 59.0 4.11 0.10 0.67 0.18 Figueiredo et al.
(2020)
Chemical sewage sludge 500 79.0 6.13 0.12 0.82 0.17 Figueiredo et al.
(2020)
Herbaceous and agricultural rice straw 500 27.9 5.63 9.94 1.05 0.47 Wang et al. (2013)
biomass rice straw 700 31.8 6.33 6.56 1.31 0.60 Wang et al. (2013)
wheat straw 500 14.5 0.70 24.0 0.90 0.31 Wang et al. (2013)
wheat straw 700 17.9 0.73 25.7 0.94 0.31 Wang et al. (2013)
maize straw 500 30.0 7.00 16.6 1.03 0.41 Wang et al. (2013)
maize straw 700 29.4 7.96 18.8 1.12 0.49 Wang et al. (2013)
rice husk 500 37.9 2.10 2.74 0.31 0.11 Wang et al. (2013)
bamboo wood 500 2.3 0.39 17.1 0.12 0.27 Wang et al. (2013)
bamboo wood 700 2.5 0.3 2.38 0.25 0.14 Wang et al. (2013)
coconut shell 500 7.3 0.72 20.4 0.33 0.21 Wang et al. (2013)
coconut shell 700 8.7 1.31 24.3 0.28 0.18 Wang et al. (2013)
Wood elm wood 500 1.1 0.19 4.97 0.26 0.06 Wang et al. (2013)
elm wood 700 1.8 0.16 3.71 0.44 0.13 Wang et al. (2013)
Pine 300 1.5 0.03 0.07 0.15 0.01 Enders et al. (2012)
Pine 450 1.5 ND 0.10 0.22 0.05 Enders et al. (2012)
ND means not detected.
transform to more stable K2CO3 through decomposition and rear et al., 2018a) is the dominant P species (Qian and Jiang, 2014; Li et al.,
rangement (Zhao et al., 2015; Chen et al., 2017a). In addition, silicon is 2018a), accounting for up to 75% of the total P (Qian and Jiang, 2014).
another essential element in the ash fraction of LCBB, especially for Transformations between different P species occur definitively, resulting
Si-rich LCBBs, such as biochars from sugarcane bagasse, rice straw and in changes in the proportion of each species. For example, Qian and
wheat straw (Guo and Chen, 2014; Wang et al., 2019; Hassan et al., Jiang (2014) found an increased amount of pyrophosphate at 400 ◦ C,
2020). Amorphous silicon can be converted to polymerized silicic acid which was caused by the transformation of organic P and the dehydra
via dehydration at lower temperatures, and further transformed to tion of orthophosphate. At higher pyrolysis temperatures, some phos
crystalline SiO2 at higher temperatures (Xiao et al., 2014). Mineral phates associate with metal ions to form insoluble P-containing mineral
components in low-temperature LCBBs are usually amorphous, more compounds such as stanfieldite (Ca4(Mg,Fe)5(PO4)6). The trans
soluble and lower in contents. In contrast, mineral components in formation and formation of insoluble P species causes the immobiliza
high-temperature LCBBs are usually crystallized, less soluble and higher tion of phosphorus in SSBB.
in contents (Xu et al., 2017).
SSBB features high levels of ash fractions, of which content is varied 5. Contaminants
with sewage sludge source. In general, residual SSBBs are lower in ash
fractions owing to the presence of rich organic matter, nevertheless, 5.1. Water-soluble compounds
digested SSBBs and chemical SSBBs are expected to contain larger
numbers of ash fractions. For instant, a high ash content of up to 80% The safety performance of water-soluble compounds derived from
has been reported in digested SSBB (Yuan et al., 2015). The high content biochars is especially significant for the purpose of soil application, as
of P in sewage sludge makes phosphorus the most abundant element in they are liable to be released into soil, which may pose potential risks to
SSBB. The P present in SSBB can exist in diverse forms, including soil ecosystems. To evaluate the safety performance of water-soluble
orthophosphate, orthophosphate monoesters, orthophosphate diesters compounds from biochars, recent studies have adopted various organ
and condensed pyrophosphate- and P-containing mineral compounds isms to reveal the potential risks of water-soluble compounds derived
(Qian and Jiang, 2014; Li et al., 2018a). Among the different P species, from biochars, generally including wheat, marine bacteria and animal
orthophosphate existing in the formation of AlPO4 and Ca3(PO4)2 (Li cells (Table 2). The toxicity of water-soluble compounds derived from
6
Table 2 for Zn and 0.03–0.27 mg/kg for As. Chen et al. (2017b) found that
The negative influence of water-soluble compounds derived from biochars on biochars derived from maize contained 1.12–1.65 mg/kg As,
organisms. 0.18–0.21 mg/kg Cd, 12.3–16.9 mg/kg Cu, 3.96–5.19 mg/kg Pb and
Feedstock Targeted Toxicity source Negative Reference 38.0–66.8 mg/kg Zn. According to the guidelines of the International
organism influence Biochar Initiative (IBI), all the contents of PTEs in LCBB were below the
Acorus Wheat Asarone Reduction in Wang et al. maximum allowed thresholds. Therefore, the environmental risks
calamus germination (2016) attributed to PTEs associated with LCBB following its application to soil
rate and length were likely to be minimal.
of shoot and
The high contents of PTEs in SSBB are a major concern for practical
root
Acorus P. aeruginosa Asarone inhibition of Wang et al. soil application. SBB were reported to contain 4410–5250 mg/kg Pb,
calamus growth (2016) 875–1090 mg/kg Zn, 86.3–103 mg/kg Ni, 123–235 mg/kg Cd,
Acorus C. elegans Asarone Increase Wang et al. 27–37 mg/kg As, 195–227 mg/kg Cu and 103–118 mg/kg Cr (Yuan
calamus C. elegans (2016) et al., 2015). Pyrolysis contributed to the enrichment of PTEs in SSBB,
mortality
Cellulose Synechococcus Mono-,di-,and Growth Smith et al.
and the enrichment of PTEs increased with increasing temperature from
trisubstituted inhibition (2016) 300 to 500 ◦ C (Yuan et al., 2015; Jin et al., 2016), because the loss in
phenolic weight of organic compounds exceeded that of PTEs. However, pyrolysis
compounds also resulted in the transformation of PTEs from relatively mobile
Miscanthus Vibrio fischeri ND Luminescence Oleszczuk
fractions to more immobile fractions (Jin et al., 2016; Xing et al., 2019),
inhibition et al.
(2013) reducing the bioavailability of PTEs in SSBB. This effect might be
Pinewood Synechococcus Acidic and bio- Growth Smith et al. ascribed to (i) the interaction between PTEs and the silicate lattice in
oil like inhibition (2016) biochar (Chen et al., 2017b); (ii) the decomposition of organic
substance ligand-complexed PTEs and carbonate-bound PTEs; and (iii) the occur
Wicker Daphnia Total 100% mortality Oleszczuk
rence of vitrification during high temperatures pyrolysis embedding
magna polycyclic rate et al.
aromatic (2013) PTEs into solid solutions (Chen et al., 2014). Xing et al. (2019) reported
hydrocarbon that the bioavailable PTEs significantly decreased from 91.65% to
Sewage Vibrio fischeri Heavy metal Luminescence Xing et al. 9.44% for Cu, from 98.82% to 63.34% for Zn, from 97.91% to 52.11%
sludge inhibition (2019)
for As, from 55.91% to 4.87% for Pb, from 78.20% to 12.50% for Cd, and
ND means not detected. from 73.51% to 9.57% for Cr when sewage sludge was pyrolysed to
biochars at 900 ◦ C. It was suggested that high-temperature SSBBs had
biochar is closely related to the biochar feedstock, pyrolysis temperature minor harmful effects in terms of heavy metals.
and type of pyrolysis reactor (Smith et al., 2012, 2016; Chen et al.,
2017b). For cellulose-based biochars, cellulose-derived intermediates, 5.2.2. Strategies for reducing PTE contents
including catechol and hydroquinone and acidic compounds, were the Co-pyrolysis of sewage sludge with some additives might be a
main sources of toxicity in water-soluble compounds (Smith et al., promising way to minimize risks from heavy metals. Plant residues
2016). Significant toxicity effects were reported to be concentrated in contain lower levels of heavy metals. The addition of plant residues and
low-temperature cellulose-based biochars, corresponding to the lower co-pyrolysis with sludge resulted in the dilution of the total contents of
pyrolysis temperature ranges of cellulose-associated intermediates. heavy metals (Jin et al., 2017). Metals in sewage sludge could also be
However, polycyclic aromatic hydrocarbons (PAHs) may account for the entrapped or chelated with some surface functional groups in plant
toxicity effects of wood-based biochars (Smith et al., 2016), which are residues, indicated by the further transformation of heavy metals to a
less dominant due to the hydrophobicity of PAHs. more stable form occluded in the oxidizable and residual fractions after
In contrast, the negative influence of water-soluble compounds co-pyrolysis of sewage sludge with plant residues (Jin et al., 2017). For
derived from SSBB was ascribed to high contents of metal ions, high instance, Jin et al. (2017) co-pyrolysed sewage sludge with bamboo at a
salinity and weak acidic pH (Mumme et al., 2018; Xing et al., 2019). The weight ratio of 1:1. The contents of PTEs in co-pyrolysis biochars were
toxicity of water-soluble compounds derived from SSBB decreased with reduced to approximately 50% with respect to the contents of metals in
increasing temperature (Xing et al., 2019). Heavy metals could be sewage sludge and bamboo biochars at the corresponding temperatures.
transformed from soluble fractions to immobilized fractions at high After co-pyrolysis at 600 ◦ C, approximately 25% of the Cu was occluded
temperatures, as heavy metals might be trapped in the carbon matrix in in the residual fraction, 3.2 times more than that in single pyrolysis
the form of organometallic complex or form insoluble inorganic com biochar. A total of 69.0–86.1% of Pb was occluded in the residual
pounds via association with minerals. High-temperature pyrolysis also fraction with increasing temperature from 400 to 600 ◦ C. According to
reduced the salinity, and the pH of water-soluble compounds tended to our knowledge, there are few available studies regarding the effects of
be neutral after high-temperature pyrolysis. To date, no evidence has co-pyrolysis with mineral compounds on lowing the bioavailability of
confirmed the contribution of organic compounds in water-soluble the inherent metals in sewage sludge-based biochars. However, it is still
compounds derived from SSBB to organism toxicity. Compared with theoretically reasonable to postulate that the addition of mineral com
metal ions, salinity and pH, organic compounds might be a secondary pounds and co-pyrolysis with sludge may result in the immobilization of
factor that results in the organism toxicity of SBB. inherent heavy metals to some extent. On the one hand, mineral oxides
such as iron oxides are well-known to generate precipitates with free
metal ions (Jiang et al., 2012), ultimately leading to the transformation
5.2. Potential toxic elements (PTEs) of heavy metals from a free state to a stable state. On the other hand, the
addition of mineral compounds was found to enhance the carbon
5.2.1. The content and bioavailability of PTEs retention and stability of biochars via physical protection from mineral
PTEs are not severe issues associated with conventional LCBBs, as the coatings on the surface of biochars (Li et al., 2014; Zhao et al., 2016).
contents of PTEs in most plant residues were very low and could be The relatively rigid carbon matrix possibly hindered the leaching of
neglected. Freddo et al. (2012) reported that the contents of PTEs in inserted heavy metals from carbon structures. In addition, the effect of
biochars from bamboo, redwood and maize were in the range of co-pyrolysis of additives with sewage sludge on immobilization of heavy
0.02–0.94 mg/kg for Cd, 0.12–6.84 mg/kg for Cr, 0.04–13.2 mg/kg for metals is still inconsistent, depending on the types of additives, blend
Cu, 0.1–1.37 mg/kg for Ni, 0.06–3.87 mg/kg for Pb, 0.94–207 mg/kg ratios, feedstock type and pyrolysis conditions. Further investigations, in
7
terms of the optimized co-pyrolysis parameters and co-pyrolysis mech vapors with solids (Buss et al., 2016), thereby limiting the formation and
anism, are needed. re-condensation of PAHs during the pyrolysis process. Recent studies
demonstrated that separating the pyrolysis gas by increasing the carrier
5.3. PAHs gas flow effectively reduced 79.72–91.88% of PAHs associated with
biochars (Buss et al., 2016; Madej et al., 2016). In addition, a change in
5.3.1. The content and bioavailability of PAHs the carrier gas from N2 to CO2 had a positive effect on reducing the total
Given the well-recognized carcinogenicity, teratogenicity and gen ΣPAHs contents and the freely dissolved ΣPAHs contents in SSBBs, as
otoxicity of PAHs, a maximum of 4 and 12 mg kg-1 16 PAHs is defined by well as on changing the profile of PAHs towards an increased proportion
the European Biochar Certificate (EBC) for premium- and basic-grade of light compounds (Konczak et al., 2019). The presence of CO2 as a
biochars, respectively. The IBI guidelines have also established carrier gas suppressed the occurrence of an addition reaction in the gas
maximum allowed values of 6 and 20 mg kg-1 16 PAHs. The total Σ PAH phase and promoted the thermal cracking of volatile chemical com
contents of LCBB are in a wide range of 50–30200 ng/kg (Keiluweit pounds derived from the thermal degradation of the feedstock (Kwon
et al., 2012; De la Rosa et al., 2019), varying with the pyrolysis pa et al., 2012, 2015). The presence of CO2 also caused the cleavage of the
rameters and types of pyrolysis reactors. Several studies have reported benzene ring and inhibited the formation of aromatic compounds (Gao
that wood-based biochars contain lower contents of Σ PAHs than et al., 2013; Kwon et al., 2015). Moreover, some studies attempted to
HAAB-based biochars. Buss et al. (2016) analysed Σ PAHs in 46 biochars decrease the contents of PAHs by means of co-pyrolysis, and the PAH
derived from different types of wood and straw. Straw-derived biochar suppression effects varied. Co-pyrolysis of sewage sludge with willow
was shown to contain 5.8 times higher PAH concentrations than was reported to contribute to a 7.0–52.3% reduction in total PAH con
softwood-derived biochar. Fabbri et al. (2012) found that biochars tents and a 15.2–39.7% reduction in the freely dissolved ΣPAHs contents
produced by slow pyrolysis from woody biomass contained the lowest associated with sewage sludge-based biochars (Konczak et al., 2019).
levels of PAHs. In contrast, De la Rosa et al. (2019) reported that the Co-pyrolysis of barley straw with iron salts suppressed formation of
feedstock characteristics had little effect on the contents of PAHs in PAHs in biochars but promoted the migration of PAHs to
biochars produced from rice husk, wood and sewage sludge using three high-molecular-weight compounds (Zhao et al., 2020).
different pyrolytic reactors and temperatures. The contents of
bioavailable PAHs tend to reflect their actual exposure risks in biochars, 6. Potential soil application
as PAHs are suggested to be strongly sorbed to the biochar matrix and
not readily desorbed from the biochar matrix (Hale et al., 2012; Hilber 6.1. Immobilization of heavy metals(loid) in soils
et al., 2017). In a survey examining the bioavailable PAHs in biochars
via the equilibrium passive sampling method, only 9 out of 29 LCBB had An increasing number of studies have shown that SSBB has an
bioavailable PAHs above the maximum blank level of 12 ng/L for the Σ outstanding performance in the immobilization of cationic metal species
16 US EPA PAHs (Hilber et al., 2017). According to existing reports, the in soils, which are mainly attributed to the rich contents of ash in SSBB.
concentrations of bioavailable PAHs in LCBB are in the range of The possible immobilization mechanisms of cationic metal species by
0.128 ± 0.0235 to 161.73 ± 71.48 ng/L (Hale et al., 2012; Hilber et al., SSBBs include (i) precipitation of cationic metal species with anions,
2017), and obviously decreased after artificial ageing (Hale et al., 2012). such as hydroxyl, phosphate and carbonate; (ii) inner-sphere complex
Sewage sludge was reported to contain inherent Σ PAHs in the range ation of cationic metal species with mineral oxides and organic carbon
of 0.251–13.833 mg/kg (Dai et al., 2014; Waqas et al., 2014; Zielińska (Fig. 5(a)) (Fang et al., 2016; Gonzaga et al., 2018). SSBBs were reported
and Oleszczuk, 2015). The inherent Σ PAHs in sewage sludge had no to effectively immobilize Pb, Zn and Cu in soils, and the abundant
direct influence on the content of Σ PAHs associated with SSBB, and phosphate in SSBB and hydroxyl were the most common ligands to
were observed to decrease or increase after sludge pyrolysis (Dai et al., precipitate with cationic metals (Fang et al., 2016; He et al., 2019;
2014; Zielińska and Oleszczuk, 2015). As mentioned above, there is still Gonzaga et al., 2020). He et al. (2019) concluded that precipitation of Pb
no clear trend indicating the influence of the feedstock on the content of and Cu with phosphate released from SSBB was responsible for the
Σ PAHs in biochars. Therefore, it is difficult to determine differences in Σ immobilization of cationic metals in soils amended by 4% SSBB. Fang
PAHs between LCBB and SSBB. The bioavailable PAHs concentration in et al. (2016) even observed the formation of lead phosphates precipi
SSBB was reported to be in the range of 81–11,750 ng/L (Zielińska and tation (e.g., K2Pb(PO3)4) on the surface of SSBB after 30-day soil incu
Oleszczuk, 2016b; Chen et al., 2019), much higher than those observed bation. Zhou et al. (2017) attributed the decreasing Zn(II)
by Hale et al. (2012) for biochars produced from plant residues. This concentrations in leachate from soils amended with SSBB to the trans
result can be explained by the fact that the lower surface area, lower formation from Zn(II) ions to Zn(OH)2 precipitation. Similarly, Gonzaga
aromaticity and lower hydrophobicity of SSBBs result in a lower et al. (2020) found SSBB could significantly decrease the contents of
adsorptive capacity for PAHs (Hilber et al., 2017; Konczak et al., 2019), mobilized Cu, but increased the content of immobilized Cu. He also
thereby causing a higher quantity of PAHs to be released from SSBBs. In ascribed immobilization of Cu to the formation of copper oxy(hydrox
addition, the interactions between the mineral phase, organic phase and ide) species. Besides, inner-sphere complexation between Pb/Cu and
PAHs also promote PAHs bioavailability to some extent. Chen et al. ferric oxides and manganese oxides in SBB are frequently reported by
(2019) found increased leaching of PAHs from SSBBs with increasing many studies. He et al. (2019) found amendment with 4% SSBB
temperature, which was accompanied by the enhanced release of hy increased reducible fractions of Pb and Cu by 9.80–12.75% and
drophobic organic compounds, calcium, aluminum and barium. It was 24.05–27.21%, respectively, which was related to the inner-sphere
explained that hydrophobic organic compounds (HOCs) created a mo complexation with Fe-Mn oxide. Fang et al. (2016) also found rapid
bile phase to facilitate the mobilization of PAHs into water, resulting in reduction in acid exchangeable Pb(II) and significant increase in
an enhancement in PAH bioavailability. Higher pyrolysis temperature reducible Pb and oxidizable Pb in soils amended by SSBBs, indicating the
could result to much destruction of HOC-(metal ion)-mineral linkages, inner-sphere complexation between Pb(II) and Fe-Mn oxide and organic
further improved the release of both PAHs and metals ions (Chen et al., carbon.
2019). Limited studies have focused on the role of SSBB in mobility and
migration of oxyanionic metals in soils, such as Cr(VI) and As(III). Redox
5.3.2. Strategies for reducing PAHs is considered to be the main mechanism that leads to the immobilization
Carrier gas has been confirmed to have a significant influence on the of oxyanionic metals in SSBB amended soils. It was reported that the
contents of PAHs associated with biochars. The carrier gas can affect addition of 1–5% SSBBs effectively reduced the total Cr and Cr(VI) levels
secondary reactions by changing the intensity and duration of contact of in soil acid batch extracts (Fang et al., 2016). A large amount of DOM
8
Fig. 5. Major mechanisms of sewage sludge-based biochars and lignocellulose-based biochars that remediate contaminants in soils. (a), inorganic contaminant; (b),
organic contaminant.
and Fe(III) released from SSBB can be served as electron donors or complexation with organic functional groups than those of Pb(II) and Cd
electron shuttles to promote Cr(VI) reduction. In addition, Fang et al. (II), due to the high stability of complexes of Cu(II) with organic func
(2016) also reported that application of SSBBs could oxidize 30.5% As tional groups (Jiang et al., 2012). The hydrolysis constant of Pb(II) and
(III) to less mobile As(V). SSBBs was found to contain rich Fe(II), which Cu(II) is lower than that for Cd(II) and Ni(II), Pb(II) and Cu(II) are easily
accounted for 33% of 30,625 mg kg-1 total Fe content. The high levels of immobilized by LCBBs via cation exchange (Uchimiya et al., 2011a). In
Fe(II) in SSBB was indicated to co-oxidize with As(III) in an aerobic addition, low-temperature LCBBs preserve many of the
environment, leading to the formation of less mobile As (V) (Fang et al., oxygen-containing functional groups originating from the feedstock,
2016). Conversely, increase in As mobility after applying SSBB in soils including hydroxyl, phenol and carboxylic acid groups. These
has also been reported by some studies (Kim et al., 2018; He et al., oxygen-containing functional groups are mainly in dissociated form and
2019). As immobilization is a complex process in biochar-soil systems, can be deprotonated in a certain range of pH, favoring the surface
which is related to Fe redox, P competition and DOM complexation. complexation and cation exchange between LCBBs and cationic metal.
More investigations are needed on the mechanisms and effects of SSBBs Deprotonated functional groups also increase the negative charge of
on As immobilization. LCBBs, promoting the electrostatic attraction between LCBBs and
LCBB has been used effectively to immobilize various cationic metal cationic PTEs. On the other hand, in high-temperature LCBB, degrada
species in soils, including Pb, Cd, Cu and Ni (Uchimiya et al., 2011a; tion of oxygen-containing functional groups results in a corresponding
Jiang et al., 2012). LCBB generally influence the mobility of cationic drop in the surface negative charge. High-temperature LCBB with
metal species through surface complexation, cation exchange, electro reduced negative charge results in less stable and dispersed colloidal
static attraction, and precipitation (Uchimiya et al., 2011a; Qian et al., particles, which is more likely to agglomerate and precipitate with
2019; Tan et al., 2020), which is highly determined by properties of cationic PTEs (Tan et al., 2020).
LCBB and types of metal element. For example, under the same condi The efficiency of pristine LCBB in immobilization of oxyanionic
tions, a higher portion of Cu(II) can be immobilized by LCBBs via surface metals is relatively low. Liu et al. (2020) reported that LCBB only
9
decreased Cr(VI) concentration in soil leachate from 62.4 mg/L to 2014). PAH degradation was generally found in soils amended with
55 mg/L. Lebrun et al. (2017) found that application of LCBBs at a 2% low-temperature LCBB or with a combination of biochars and exogenous
and 5% dosage had no effect on As immobilization. Lomaglio et al. carbon sources (Ni et al., 2017), this process was delayed compared with
(2017) even observed that LCBB addition in contaminated mine soils PAHs immobilization. More residual bio-oil was attached to the surface
increased As concentration in soil leachate by 33% and 70% for 2% and of low-temperature LCBB than high-temperature LCBB produced from
5% biochars, respectively. It is due to increase in soil pH induced by the same feedstock. Abundant bio-oil and exogenous carbon sources
LCBBs that promote competition between hydroxyl and oxyanionic could serve as metabolic substrates to stimulate the growth and activity
metals for binding sites, as well as electrostatic repulsion between of PAH degraders.
oxyanionic metals and electron-negative biochars. To improve oxy
anionic metals immobilization, many studies have tried to modify LCBBs 6.3. Nutrient input
with Fe-containing mineral compounds. Liu et al. (2020) loaded
Fe2(SO4)3 on the LCBBs to synthesize zerovalent iron The high ash content of SSBB indicate that SSBB can improve soil
nanoparticles-LCBB composites. The composite biochars could fertility by releasing inherent mineral fractions into soils. The abundant
completely remove 62.4 mg/L Cr(VI) from soil leachates. Yin et al. phosphate in SSBBs can rapidly promote the increment of soil fertility.
(2017) loaded Fe oxides on the surface of LCBBs. The Fe-LCBBs reduced For example, Yue et al. (2017) found that application of SBBs increased
approximately 50% soluble As in soil porewater, which was ascribed to soil available P by up to 38 times. In addition, SSBB was found to have a
the high affinity of As on Fe oxides. slow phosphorus release effect due to its high levels of medium-term and
long-term plant available P pool. Figueiredo et al. (2020) conducted a
6.2. Immobilization and degradation of organic compounds in soils four-year assessment to study the effects of chemical SSBBs on soils P
pool. In the two first years, it was found that chemical SSBBs increased
Limited research has reported an effective role of SSBB in the soil total P content and inorganic P content by approximately 2.4 and 2.5
immobilization of organic compounds in soils. The addition of 5% SSBB times, respectively. Chemical SSBBs also increased soil available P by a
was reported to decrease the bioavailability and bioaccessibility of Σ factor of 8.5 times in the first cropping season. Even in the two last
PAHs in soils by 27.0–71.6% and 14.2–55.8%, respectively, and the cropping seasons, soil available P was still maintained 7.4 times levels.
result was highly dependent on the soil type and biochar applied (Zie LCBB contains a high content of carbon and low ash content. The
lińska and Oleszczuk, 2016a). Soil amendment with 700 ◦ C SSBB addition of LCBB can input a large amount of organic C into soils (Wang
showed greater immobilization effectiveness than amendment with et al., 2015b). Moreover, certain LCBBs contain high levels of silicon and
500 ◦ C SSBB, which was ascribed to the more developed porous struc can be utilized as potential alternate silicon sources for the growth of
ture, higher content of aromatic structures (H/C) and higher degree of plants. For example, Wang et al. (2019) investigated the soil Si cycle and
hydrophobicity (O/C) of 700 ◦ C SSBB than 500 ◦ C SSBB (Fig. 5(b)). It plant uptake of Si in a soil-rice system amended with Si-rich biochars
was indicated that physical adsorption and π-π electron interactions derived from rice straw. Rice straw derived biochars increased the total
were the dominant immobilization mechanisms in the interaction be uptake of Si in rice plants by 10.33–61.48%, which was derived from
tween SSBB and PAH-polluted soils. Among these interactions, the both soil Si and biochar Si. The contribution of soil Si to total Si uptake in
graphitic structures in biochars could serve as π-electron donors to rice plants was decreased by applying rice straw-derived biochars,
enable π-π interactions with compounds with benzene rings, regarded as indicating that most of rice Si uptake were from biochar Si. Therefore, it
electron-deficient groups. Therefore, π-π interactions generally tend to could be concluded that biochars could release Si into soil and partici
present in biochars at higher temperatures. Moreover, low-temperature pate in soil silicon cycle in the soil-rice system. Given the low mineral
SSBB contains higher levels of DOC, which can combine with PAHs to content of LCBBs, plant residues have been co-pyrolysed with mineral
inhibit sorption or promote the desorption of PAHs in soils (Kopinke fertilizer to produce appropriate biochars for fertilization. For instance,
et al., 2011; Tang et al., 2016). Currently, although high proportions of Gao et al. (2020) produced biochars co-pyrolysed from plant-based
the ash fraction were confirmed to indirectly influence the sorption biomass with orthophosphate at 500 ◦ C, and 3% co-pyrolysis biochars
behavior of organic compounds by changing the spatial arrangement of were applied into soils. Consequently, soil available P was significantly
the biochar carbon fraction and the formation of aromatic structures in increased by adding co-pyrolysis biochars. During co-pyrolysis process,
the liquid phase (Xu et al., 2017), it is still unknown whether a high ash interaction between plant residues and mineral fertilizer can also result
fraction in SSBB would directly or indirectly impact the bioavailability in the formation of organic-mineral complex and precipitate, reducing
and bioaccessibility of organic compounds in soils. For example, in a release rates of mineral fertilizer. Therefore, the composite biochars
long-term study, the ageing effect might induce the leaching of ash feature a higher nutrient content and a lower release rate and can be
components with prolonged contact time, leading to the improved considered slow-release fertilizers.
sorption capacity of SSBB due to the unblocking of biochar pores. It can be inferred that the feedstock and pyrolysis temperatures
Compared with SSBB, LCBBs were observed to be more effective at determine the contents and species of nutrient elements, subsequently
reducing organic compound bioaccumulation (Khan et al., 2015). This affecting their potential as fertilizers. However, the effect of nutrient
effectiveness was because the ability of biochar to sorb organic com input has been shown to be highly variable in practical applications,
pounds is highly dependent on the graphene-like carbon fraction and the depending on the application rate of biochar, soil pH and soil cations
non-crystalline amorphous carbon fraction in the biochar, which are and anions (Glaser and Lehr, 2019; Figueiredo et al., 2020). In general,
involved with partitioning, hydrophobicity, and π-π electron in the appropriate application of SSBB with a high ash content to sandy
teractions (Xu et al., 2017) (Fig. 5(b)). LCBBs were characterized by a soils or acidic soils is highly recommended for improving soil nitrogen
rich carbon fraction and lower O/C ratio and were regarded as a priority and phosphate fertility. Lower soil pH contributed to the abundant
3+
amendment for immobilizing organic compounds in soils. In a green release of NH+ 4 , PO4 and K but suppressed the release of dissolved Si
+
house experiment that investigated the influence of various biochars on via the formation of insoluble Si-containing compounds. Large amounts
the bioaccessibility of PAHs in soils, the reduction in the accessible Σ 16 of Ca2+ and Mg2+ in soils could produce precipitates with P2O7,
PAHs was from 68% to 80% for biochars derived from peanut shells, reducing the release of pyrophosphate.
which was significantly higher than that in SSBB (27–46%). In addition,
LCBB was found to indirectly impact the total contents of Σ 16 PAHs and 6.4. Soil quality enhancement
their bioavailability through microbial biodegradation (Ni et al., 2017).
The usual PAH degraders include Arthtobacter, Flavobacterium, Betapro A common consensus has been reached in that the high content of
teobacteria and Gammaproteobacteria (Martin et al., 2012; Xu et al., ash in SSBB has positive effects on improving the quality of acidic soil by
10
increasing the soil pH and alleviating of Al toxicity (Waqas et al., 2014). carbon sequestration.
Pyrolysis results in the transformation of cations (K, Ca and Mg) to The actual persistence of biochars in soils is complicated by many
carbonates, hydroxides and oxides. These mineral fractions either are factors. Contact between soil minerals and biochars is conductive to the
inserted into the structure of the biochar, or dissolve in soil pore water formation of organometallic complexes, which are capable of physically
and then bind with H+ ions to neutralize soil acidity. In addition, min preventing O2 accessibility and reducing biochar reactivity from
eral fractions, such as silicon, calcium and phosphate, can form com chemical and biological oxidation (Yang et al., 2016). Conversely, the
plexes with exchangeable Al in soil. However, the liming effect was not addition of biochars might promote the enrichment of microbes capable
limited to SSBB, but was also frequently observed in soils amended with of utilizing recalcitrant carbon sources. The presence of high proportions
LCBB (Hartley et al., 2016). To date, the differences in the liming effect of gram-positive bacteria in soil promoted the biodegradation of bio
between SSBB and LCBB have not been comprehensively elucidated. The chars (Sheng et al., 2016). In addition, the co-metabolic effects of mi
liming effect of biochars is related to ash fractions, surface functional crobes induced by the additional input of plant residues accelerate the
groups, application rates of the biochar and soil type. mineralization of biochar (Keith et al., 2011; Sheng et al., 2016). Some
Biochars can provide biological available carbon sources for soil environmental factors, such as soil moisture, ambient temperatures and
microbes to stimulate microbial biomass and impact microbial com soil pH, also influence the persistence of biochars (Singh et al., 2012).
munity structure (Chen et al., 2016; Yang et al., 2019a; Zhang et al., Therefore, these factors need to be considered when applying biochars
2020). Especially for sewage sludge-based biochars, a high content of in soil with different biochemical properties to investigate their stability.
aliphatic carbon, as indicated by a higher H/C ratio is significant for soil
microbial growth and metabolism. In contrast, high levels of refractory 7. Economic feasibility
lignin present in wood-based biochars mean less release of DOC into
soils (Kim et al., 2020). In a study investigating the effects of biochars on The significant factors for the biochars to evaluate their economi
soil microbial activities and soil DOC, a positive correlation between cally feasible application are economic cost, as well as agronomic and
DOC and activities of microbes was revealed by Yang et al. (2019a). In environmental benefits. The cost of biochars includes capital cost,
addition, as microbes have different metabolism capacities of carbon feedstock cost, production cost, maintenance cost, labor cost and storage
sources, only a certain part of biochar-derived DOM can be available for cost (Ahmed et al., 2016; Shahbeig and Nosrati, 2020), being it strongly
specific microbes. For example, aliphatic compounds from biochars depending on local availability, processing required, preparation con
were responsible for the increasing biomass of Dyadobacter, Sphingo ditions and both recycle and lifetime issues. The agronomic and envi
bacterium and Novosphingobium, while Methylotenera, Acinetobacter and ronmental benefits of biochars can be directly quantified by calculating
Reyranella were reported to prefer to utilize highly aromatic crops yields and estimating net global warming potential (GWP). The
combustion-derived condensed polycyclic aromatics (Zhang et al., additional values of biochars, including waste management and
2020). Given the differences in hydrophobicity and aromaticity between reducing requirements of fertilizer and liming, can further improve the
SSBB-derived DOM and LCBB-derived DOM, it can be inferred that SSBB economic values of biochars.
and LCBB may change the microbial community structure towards The high moisture content of sewage sludge requires dewatering
opposed ways. Changes in microbial biomass and microbial community pretreatment process before pyrolysis, which causes a relative high
structure are highly related to the improvement of soil quality. Soil equipment cost and power consumption. Shahbeig and Nosrati (2020)
microbes, such as arbuscular mycorrhizal fungi, can promote the for conducted a techno-socio-economic assessment for a designed sludge
mation of soil microaggregation via the secretion of extracellular mac pyrolysis plant assumed to sell all the pyrolysis products, including
romolecules (King, 2011), which is helpful for the improvement of soil bio-oil, bio-gas and biochar. The total capital cost of SSBB was the sum of
physical structures and soil pore water retention. cost of dewatering, drying, storage tank, pyrolysis reactor, cyclone and
condenser, roughly equal to €19,387. The dewatering unit accounted for
6.5. Carbon sequestration 6% of the main equipment costs. The negative present value of the py
rolysis plant was estimated to be €217,305 over 20-year project period,
LCBB exhibits good performance in soil carbon sequestration indicating the economic feasibility of sludge pyrolysis. Sewage sludge is
(Grutzmacher et al., 2018). For example, only 6% of the initially added produced as a waste in high amounts. The easy availability of sewage
biochars originating from Lolium residues were mineralized to CO2 sludge and high yields of SSBB lower the costs and minimum product
during the 8.5-year incubation in soils (Kuzyakov et al., 2014). Under selling prices (MPSP) of SSBB, indicating its economically advantages in
controlled soil incubation conditions, biochars derived from eucalyptus wide application.
sawdust showed a lower C mineralization rate than sewage sludge-based Lignocellulosic biomass needs to be washed, dried and rived before
biochars (Grutzmacher et al., 2018), indicating the high carbon pyrolysis. The washing, dryer and shredder equipment account for 2%,
sequestration ability of LCBB. In contrast, the carbon stability of SSBB 7% and 9% total equipment costs (Giwa et al., 2019). Compared with
was lower. The carbon structures of biochars affect the persistence of SSBB, LCBB has a higher feedstock cost and a higher MPSP value (Cheng
biochars in soil, thereby influencing the ability of biochar to sequester et al., 2020). In contrast, LCBB produced at higher temperatures deliver
carbon (Singh et al., 2012; McBeath et al., 2014). The stable polycyclic much more negative GWP than that of SSBB (Cheng et al., 2020), indi
aromatic carbon content determines the persistence of biochars, which cating environmentally superiority of high-temperature LCBB that
was found to be high in wood-based biochars. However, the formation of partly offsets the feedstock cost of LCBB. Joseph et al. (2020) performed
stable polycyclic aromatic carbon compounds is retarded in feedstock a cost-benefit analysis of wood-based biochars application to improve
with high ash contents. Moreover, Grutzmacher et al. (2018) confirmed avocado yields in a farmland, in which they calculated the net present
a direct correlation between the cumulative CO2 emissions of biochars value (NPV) by assuming sustaining yields surplus of fruit trees and
and the C/N ratios. The higher C/N ratio of wood-based biochars than stable avocado prices in three years. The initial cost outlay of LCBB
residual sewage sludge-based biochars could explain the lower C application was US$10,770 ha− 1. LCBB application resulted in NPV of
mineralization rate of the former. Srinivasan et al. (2015) explored the US$8581 ha− 1. Hence, benefit-cost ratio was positive, indicating the
potential applications of biochars derived from different feedstocks payback period of four years.
under the same pyrolysis conditions. The H/C ratios, O+N/C ratios and
13
C Nuclear magnetic resonance (NMR) spectra all confirmed that there 8. Major challenge and future perspectives
are higher aromatization degree and more condensed aromatic struc
tures in wood-based biochars than residual sewage sludge-based bio In the aforementioned analysis, differences in pyrolysis processes
chars, suggesting great potential of wood-based biochars for use in and various fractions between lignocellulose-based biochars and sewage
11
sludge-based biochars were critically discussed. Various performance pyrolysis temperature ranges and various pyrolysis technologies. The
metrics related to soil application, including carbon sequestration, unclear impact of feedstock and pyrolysis parameters on certain char
nutrient input, soil quality enhancement and inorganic/organic acteristics of biochar, such as biochar-derived DOM, also complicate the
pollutant immobilization, of lignocellulose-based biochars and sewage selection of an appropriate biochar. In addition, the same type of biochar
sludge-based biochar were also summarized. However, some key issues may have different effects on different types of soils. For example, bio
remain unclear with respect to selecting appropriate types of biochars chars were reported to significantly reduce the porewater Zn, Pb and Cd
for distinct proposed uses in soils, which is of significance for the concentrations in acidic mine soils but showed no consistent effects on
effective and extensive application of biochars in soils. the porewater Zn, Pb and Cd concentrations in basic mine soils (Alvar
First, limited information is available on the contents and molecular ez-Rogel et al., 2018). The differences in soil characteristics may influ
characteristics of biochar-derived DOM, with respect to variations in ence the effects of the biochars on reducing porewater metals
feedstock and pyrolysis parameters. The interaction mechanisms be concentrations. The interactions between biochars and soil minerals can
tween biochar-derived DOM and soil microorganisms, iron/manganese influence the pore structure of biochars, the speciation of the ash frac
oxides and contaminants are still unclear, but this is an important aspect tion in biochars and morphology of the biochar carbon structure, which
that needs to be further considered. For example, biochar-derived DOM will influence the effects on contamination immobilization, nutrient
can increase Cu and Cd mobility through complexation with phenolic, input and C sequestration to varying degrees (Qian et al., 2013; Yang
carboxyl amide and thiol groups (Huang et al., 2019; Xing et al., 2020). et al., 2016; Kumar et al., 2018). However, no standard has been
The interaction between iron oxides and biochar-derived DOM cause developed to classify biochars with various characteristics. The in
reductive dissolution from Fe oxides to Fe(II), which could result in the teractions between biochars and soils are still unclearly clarified. The
desorption of As from iron oxides (Kim et al., 2018). Biochar-derived lack of systematic matching between soil types and different biochars
DOM stimulates microbial activity through the breakdown of labile has also exacerbated difficulties in the selection of appropriate biochar.
soluble organic carbon. The enhancement of microbial activity may Accordingly, future biochar research should emphasize the in-depth
promote the formation of soil aggregates via the secretion of extracel understanding of the ecological roles of biochar-derived DOM, espe
lular macromolecules (King, 2011). However, how and to what extent cially regarding the interaction among biochar-derived DOM, soil mi
can biochar-derived DOM affect the formation of soil aggregates and the crobes and soil pollutants, which are closely related to the
transport and fate of soil contaminants? What are the conditions under biogeochemical cycle of carbon, transportation of contaminants and
which soil microorganisms participate in interactions with improvement of soil quality. It is also necessary to establish a more
biochar-derived DOM and affect the ecological roles of biochar-derived realistic risk assessment of the potential exposure of biochar-associated
DOM? Overall, the net effects of DOM released from biochars are not yet toxic fractions. Effective and innovative technologies to lower the con
fully understood due to insufficient data on the relationships between tents of the toxic fractions of biochars and control their release are
the characteristics of biochar-derived DOM and its interactions with needed; such technologies can be explored from the aspects of the se
various soil components. lection of optimal feedstock, optimization of preparation parameters
Second, biochar-associated toxic fractions are still the major defect and suitable scopes of application. Much attention should be paid to
that impedes the wide application of biochars, especially SSBB, whose develop classification of characteristics of biochars and to clarify the
feedstocks contain high levels of PTEs and PAHs. Although IBI and EBC interactions between soils and biochars. Systematic matching between
have established maximum allowed values for corresponding contami soil types and different biochars based on distinct purposes of use needs
nants, the soil application of biochar is a long-term process, and the to be established as soon as possible.
potential influence of the long-term accumulation of contaminants
carried by biochars is worth considering. In addition, the rationality of 9. Conclusion
IBI and EBC guidelines needs to be considered urgently. For example,
5.33 mg/kg and 5.65 mg/kg Σ 16 PAHs were detected by De la Rosa As summarized in this review, significant differences exist in the
et al. (2019) in vineyard wood-based biochars and rice husk-based pyrolysis processes and various fractions between lignocellulose-based
biochars, respectively, corresponding to basic quality according to biochars and sewage sludge-based biochars, which play vital and
EBC guidelines. However, the total toxic equivalent concentration diverse roles in soil applications. Lignocellulose-based biochars are
(TTEC), an indicator used to evaluate the environmental risk of biochar, characterized by high aromaticity, high C contents and low ash, favor
showed that the environmental risk of vineyard wood-based biochars carbon sequestration, heavy metal retention, organic matter immobili
was twelve times lower than that of rice husk-based biochars. Therefore, zation and biodegradation. Sewage sludge-based biochars have high
it is indicated that the quality thresholds based on Σ 16 PAHs proposed levels of mineral components. Soil application of sewage sludge-based
by EBC and IBI are probably less appropriate than the use of TTEC. In biochars is a promising approach to improve soil fertility through the
addition, some emerging contaminants carried by biochars, such as toxic release of available mineral nutrients and immobilization of heavy
dissolved organic matter and environmentally persistent free radicals metals. The large amount of dissolved organic carbon in sewage sludge-
(EPFRs), should be taken into consideration. Phenolic components based biochar also suggest its potential role in the formation of soil
released from biochars were responsible for potential toxicity to fresh aggregates and interactions between DOC and soil microbes. However,
water blue-green algae (Smith et al., 2016). EPFRs detected in biochars the environmental risks related to the soil application of biochars should
were reported to have a negative influence on plant germination, shoot not be overlooked. More research is still required on in the form of in-
and root elongation, plasma membrane integrity and neurotoxicity (Liao depth investigations of the ecological roles of biochar-derived DOM,
et al., 2014; Lieke et al., 2018). However, little attention has been paid to the exploration of technologies to increase the safety performance of
the detection and management of biochar-related emerging biochars and the establishment of matching between various types of
contaminants. biochars and soil types.
Third, despite the large volume of information available on the
application of various types of biochar for the purpose of carbon Declaration of Competing Interest
sequestration, soil fertility improvement and soil contaminant immo
bilization, it is extremely challenging to select an appropriate biochar to The authors declare that they have no known competing financial
solve a targeted soil issue. The application effects depend on the char interests or personal relationships that could have appeared to influence
acteristics of the biochar, types of soil and interactions between the the work reported in this paper.
biochar and soil. Significant variability can be found in the character
istics of biochars due to the extensive sources of feedstocks, wide
12
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Ecotoxicology and Environmental Safety 208 (2021) 111756

Contents lists available at ScienceDirect

Ecotoxicology and Environmental Safety

Comparison of pyrolysis process, various fractions and potential soil

Lignin is a complex polymer of phenylpropane units comprised of 3. Carbon pool

LCBB contains a lower ash fraction in the range of 1.1–37.9%

ND means not detected.

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