Journal Pre-proofs

Preparation and application of magnetic biochar in water treatment: A critical

review

Xiangping Li, Chuanbin Wang, Jianguang Zhang, Juping Liu, Bin Liu, Guanyi
Chen

PII: S0048-9697(19)34839-9
DOI: https://doi.org/10.1016/j.scitotenv.2019.134847
Reference: STOTEN 134847

To appear in: Science of the Total Environment

Received Date: 3 July 2019

Revised Date: 29 September 2019
Accepted Date: 4 October 2019

Please cite this article as: X. Li, C. Wang, J. Zhang, J. Liu, B. Liu, G. Chen, Preparation and application of magnetic
biochar in water treatment: A critical review, Science of the Total Environment (2019), doi: https://doi.org/10.1016/
j.scitotenv.2019.134847

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 Preparation and application of magnetic biochar in water treatment: A critical

review

Xiangping Lia,b,c, Chuanbin Wanga, Jianguang Zhangd, Juping Liua, Bin Liuc, Guanyi

Chena, e,*

a China-Australia Centre for Sustainable Urban Development/ School of Environmental Science and

Engineering, Tianjin University, Tianjin 300350, PR China

b Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development,

Guangzhou 510640, PR China

c Qingdao Institute for Ocean Technology of Tianjin University, Qingdao 266235, PR China

d School of Petroleum Engineering, China University of Petroleum (East China), Qingdao, Shandong

266580, PR Chinae Tianjin Key Lab of Biomass/Wastes Utilization, Tianjin 300354,PR China

* Corresponding authors. Tel. 022-27401929. E-mail addresses: [email protected] (X.P. Li);

[email protected] (G. Y. Chen)

Abstract

In recent years, magnetic biochar has been widely used in removal of pollutants

from water. In this paper, the preparation technologies of magnetic biochar are

analyzed, and the performance and application of magnetic biochar in removal of

inorganic pollutants such as heavy metals, and organic pollutants are investigated.

Moreover, the adsorption behaviors, the key influencing factors and the adsorption

mechanisms of magnetic biochars are summarized in this paper. Compared with

common biochar, magnetic biochar is more effective in removal of water pollutants,

including Cd(II), Pb(II), Zn(II), Cu(II), methylene blue, tetracycline, pesticide and

1
phosphate. Langmuir and Freundlich models are adopted as the mainly adsorption

isotherms, while pseudo-second-order model is employed as Kinetic model of heavy

metal ions and organic contaminants in water. This study also investigates

degradation of organic contaminants in water using magnetic biochar as catalyst.

Results showed that encapsulated γ-Fe2O3 nanoparticles enhanced the catalytic ability

of persulfate activator. Further researches on preparation and application of magnetic

biochar in water treatment are prospected in this review.

Keywords: magnetic biochar, preparation, adsorption, degradation, water pollution,

contaminants

1. Introduction

As is known that about 71 % of the Earth’s surface is covered by water, but only

2.5 % of the earth’s water is fresh (Rajasulochana and Preethy, 2016). More

unfortunately, this few portion of fresh water is being polluted and destroyed

(Azizullah et al., 2011). Up to now, more than 2.3 billion people worldwide are

suffering from water-related diseases, especially for those in developing countries

(Wang and Yang, 2016). The contaminants in water include but not limited to heavy

metals, polyaromatic hydrocarbons and dyes. Once these contaminants exceed a

certain concentration in drinking water, the drinking water is no longer suitable for

drinking (Gumpu et al., 2015; Sajid et al., 2018; Wong et al., 2017). In order to

decrease the environmental hazards, various kinds of techniques have been developed

to remove contaminants from water, soil and wastewater (Groß et al., 2017; Ye et al.,

2019a; Ye et al., 2019b; Ye et al., 2017a; Ye et al., 2017b). Adsorption method is

2
found more suitable for removal of various aquatic pollutants (Haddad et al., 2019;

Khataee and Kasiri, 2010; Xu et al., 2019). With the advantage of simple processing,

low cost and high efficiency, adsorption method has attracted wide attention and has

been considered as the most common technology for removal of aquatic pollutants

(Haddad et al., 2019; Khataee and Kasiri, 2010; Nadeem et al., 2014; Xu et al., 2019).

Biochar is a kind of low-density charred carbon material, which is produced by

thermal decomposition biomass in the presence or absence of oxygen (Beesley and

Marmiroli, 2011; Regmi et al., 2012; Yuan et al., 2011). Biochar is characterized by

porous structure, large specific surface area, abundant mineral components and

surface functional groups (Tan et al., 2015). There are a wide range of raw materials

for biochar production, such as giant reed (Zheng et al., 2013), peanut husks (Cheng

et al., 2016), cotton straw (Wang and Liu, 2017), water hyacinth (Zhang et al., 2015a).

Biochar has been applied in many areas, especially used as an adsorbent in removal of

water pollutants such as Cd (Cui et al., 2016), Pb (Wang et al., 2017d), Cu (Wang et

al., 2015a), As (Zama et al., 2017), Zn (Xu et al., 2013), sulfamethoxazole (Yao et al.,

2012) and salicylic acid (Karunanayake et al., 2017).

Many efforts have been carried out to improve the adsorption capacity of biochar

(Ding et al., 2016). However, due to the small particle sizes and lower density, the

separation and reuse of biochar after adsorbing water pollutants remain one of the

major problems to be solved. Magnetic biochar is synthesized by magnetic medium

(eg. Fe (Li et al., 2017c), Fe2O3 (Zhu et al., 2014) or Fe3O4 (Shan et al., 2016)) and

biochar (Qin et al., 2017) via either pyrolysis activation or chemical co-precipitation.

3
Magnetic biochar shows excellent performance in adsorbing the pollutants from water

and can be isolated easily by using external magnets. Therefore, it has been widely

applied as an adsorbent for treating polluted water and separating small particles from

water (Li et al., 2017b; Liu et al., 2019).

This work is to review the application of magnetic biochar in removal of

contaminants from aqueous systems. The contents of this paper can be described from

following aspects: (1) the recent development progresses in the preparation and

characterization of magnetic biochar; (2) the development of magnetic biochar as an

efficient adsorbent; (3) the main factors influencing magnetic biochar’s property; (4)

the adsorption mechanisms of magnetic biochar. The purpose of this work is to

highlight the further research areas of magnetic biochar, and discuss the novel

researches of magnetic biochar materials that are possibly to be applied in wastewater

treatment.

2. Preparation of magnetic biochar

Three kind of methods are usually used to prepare magnetic materials, namely,

calcination, co-precipitation and pyrolysis method (Thines et al., 2017b). Commonly,

the typical pyrolysis process can be subdivided fast pyrolysis, slow pyrolysis and

flash pyrolysis. The corresponding operating conditions and the overall yield of

different pyrolysis types are listed in Table 1. Co-precipitation is to add precipitant to

make ions precipitate. Calcination is a thermal treating process, in which materials are

heated under certain temperature without fusion to drive off H2O, CO2, SO2 and other

volatile constituents (Thines et al., 2017b).

4
Table 1

The operating conditions and the overall yield of different pyrolysis (Laird et al., 2009; Thines et

al., 2017b).

Operating conditions Residence Pyrolysis Heating Overall yield (%)

and the overall yield time(s) temperature(K) Rate(K/s) Biochar Bio-oil Biogas

Conventional 450-550 550-950 0.1-10 35 30 35

Pyrolysis

Fast pyrolysis 0.5-1.0 850-1250 10-200 50-70 10-30 15-20

Flash pyrolysis < 0.5 1050-1300 < 1000 60 40 5-15

The three synthesis methods have their own advantages and disadvantages.

Co-precipitation has the advantages of shorter process, simple reaction conditions and

higher product purity. The calcination method is relatively simple, which employs

autoclave heating to produce magnetic biochar. In contrast, traditional heating

methods require heavy mechanical systems and inert gas to create an inert atmosphere

for magnetic biochar production.

3. Magnetic biochar in water treatment

3.1. Factors affecting the adsorption of pollutants by magnetic biochar

As shown in Fig. 1, the main factors influencing the adsorption efficiency of

magnetic biochar include pyrolysis temperature, material type, modifier type, dosage

of adsorbent, pH value, reaction temperature, contact time, initial pollutant

concentration and competitive anion.

5
 Adsorption
temperature

concentration of pollutant

impregnation ratio
Adsorption of

Chemical
pollutants in water
Initial

by magnetic
biochar

Dosage
of adsorbent

Fig. 1. Factors affecting the adsorption of pollutants by magnetic biochar

3.1.1. Effect of chemical impregnation ratio on the removal of pollutants

Ratio of raw material to magnetic material during impregnation process affects

the carbon yield and adsorption. Yap et al. evaluated the adsorption of heavy metals

by magnetic biochar under different impregnation ratios of raw material to magnetic

material (Yap et al., 2017). The results showed that the carbon yield increased from

67.37 % to 88.98 % with the impregnation ratio of raw material to magnetic material

increasing from 0.25 to 0.50. However, once the impregnation ratio was higher than

0.50, the adsorption amount of heavy metal and carbon production decreased. When

the ratio of biochar to FeCl3 was 0.5, the optimum adsorption capacity of magnetic

biochar and the highest yield of coconut shell-derived activated biochar were obtained.

During this experiment, the infused iron solution varied within the range of

6
0.01-0.1mol/L. Son et al. found that the removal efficiency and recovery rate of Cu(II)

showed the opposite trend with the load intensity of Fe (Son et al., 2017). As the iron

concentration in the loading solution increased, the removal capacity of copper by

magnetic biochar decreased. The removal efficiency of mercury by magnetic biochar

was investigated as well (Yang et al., 2016). It was reported that that the Hg0 removal

efficiency increased significantly by increasing the mass ratio of FeCl3 to sawdust,

which might be due to the fact that activated FeCl3 made certain functional groups

appear in magnetic biochar (Yang et al., 2016).

The effect of Zero-valent iron (ZVI) to biochar ratio in Zero-valent iron magnetic

biochar composites (ZVI-MBC) on the removal rate of pentachlorophenol (PCP) in

wastewater was investigated (Devi and Saroha, 2014). It was found that when the

ratio of ZVI to biochar increased from 1: 0.5 to 1: 2, the removal rate of PCP

increased from 90.1 % to 97.45 %, which was due to the enhanced dispersivity of ZVI

on biochar. However, as the ZVI-biochar ratio further increased from 1: 2 to 1: 3, the

removal efficiency of PCP started to decrease. This may due to that the excess

biochar entrapped the ZVI particles, thus preventing the direct contact between ZVI

and PCP in water and thus reducing the removal efficiency of ZVI-MBC (Dou et al.,

2010). Zhou et al. prepared eight types of ZVI biochar composites through changing

the BB:C:Fe mass-to-weight ratio of the composites. The results showed that effective

removal of As(V) and P was attributed to anionic and composite surfaces of ZVI

biochar (Zhou et al., 2014). ZVI-MBC has excellent ability to remove various

contaminants such as heavy metals, phosphates and methylene blue (MB) in aqueous

7
solution.

The optimum ratio of biochar to FeCl3 can also promote the development of

pores, which can lead to a significant increase in specific surface area and pore

volume. The influence of chemical impregnation ratio on the removal of water

pollutants by magnetic biochar is complex, separate analysis for each magnetic carbon

sample is necessary.

3.1.2. Effect of pyrolytic temperature on the removal of pollutants

The porous structures of magnetic biochar can be improved by increasing the

activation temperature or activation time, and the activation temperature was found to

play a key role (Zhang et al., 2015c).

Li et al. investigated the impact of pyrolysis temperature on the adsorption

characteristics of biochar and the corresponding adsorption behavior of aromatics

pollutants (Li et al., 2017b). The results showed that the carbonation of magnetic

biochar was enhanced with the increase of pyrolysis temperature. Magnetic biochar

with maximum surface area and pore volume was obtained when pyrolysis

temperature was 873 K. The adsorption of Congo red (CR) by magnetic biochar

prepared at different temperatures (773-1173 K) was investigated (Thines et al.,

2017a). The results showed that the removal rate of CR increased by using magnetic

biochar prepared at higher temperature, and the highest removal rate of CR was

obtained by using magnetic biochar prepared at 1073 K. However, further increasing

the preparation temperature of magnetic biochar led to the decrease in adsorption

capacity of CR. Further increase of pyrolysis temperature could lead to structural

8
damage, decrease in porosity and surface area, thus influencing the adsorption

performance (Mubarak et al., 2014). Zhang et al. found that magnetic biochar

prepared by pyrolysis of water hyacinth at 723 K (MW450) had a lower As (V)

removal efficiency than that prepared at 523 K (MW250). 95 % As(V) was absorbed

by MW250 and 79 % As(V) was absorbed by MW250 at initial As(V) concentration

of 4.946 mg/L. This is probably due to the adsorption competition between As (V)

and OH- derived from the higher mineral ash produced at higher pyrolysis

temperature, the stronger electrostatic repulsion against As(V) anions at higher pH

and the lower surface area of MW450 (Zhang et al., 2016).

The pyrolysis temperature affects the physical and chemical properties of

magnetic biochar, thus affecting the removing efficiency of pollutants in water.

Increasing pyrolysis temperature within the lower temperature range can enhance the

adsorption of pollutants by magnetic biochar.

3.1.3. Effect of pH on the removal of pollutants

The pH of solution is one of the key factors influencing the adsorption of

pollutants in water. With a lower pH range, the removal rate of pollutants can be

increased by increasing the pH of solution. The removal rate of pollutants was

decreased once the pH of solution exceeded the optimum value. The optimum

solution pH for pollutants removal varied with the pollutant and the magnetic biochar

(Cho et al., 2016; Ifthikar et al., 2017; Kołodyńska et al., 2012; Kong et al., 2017;

Lalhmunsiama et al., 2017; Li et al., 2017a; Zhang et al., 2016).

When magnesium ferrite/biochar magnetic composites (MFB-MCs) was used to

9
remove phosphate from water, it was found that when the pH of solution was higher

than the point of zero-charge (pHpzc), the surface charges of MFB-MC were

deprotonated, and a strong electrostatic repulsion was generated between MFB-MCs

and the phosphate. The pHpzc of MFB-MCs was reported to be about 8.5 (Jung et al.,

2017). In addition, the concentration of OH- was higher in solution with higher pH,

which enhanced the competition between OH- and phosphate at the binding sites.

When the pH of solution was lower than the pHpzc, the charge of MFB-MCs on the

surface was protonated, and the electrostatic attraction between MFB-MCs and

phosphate increased with the decrease of solution pH. Therefore the adsorption

capacity and removal efficiency of MFB-MCs were higher at pH=3.0 than that at

pH=5.0 and 7.0 (Jung et al., 2017).

In the study of removing MB using a novel magnetic carbon nanocomposite as

adsorbent, it was found that the adsorption capacity of MB increased from 1.31 to 16

mg/g as the pH of solution increased from 2 to 8.8, indicating that higher pH was

more favorable for MB adsorption. The lower adsorption capacity under acidic

conditions could be due to the protonation of the acidic functional groups as well as

the competition for adsorption sites between hydrogen ions and MB (Mallampati et al.,

2015; Sharma et al., 2013). The adsorption behavior of Cd(II) from rape straw by

magnetic biochar under aqueous solution was investigated. The results showed that as

the pH of the initial solution increased from 2 to 4, a dramatic increase in removal

efficiency was observed (Li et al., 2017a). When pH>5, the competition between

Cd(II) and proton for binding sites decreased with the increase of solution pH, and the

10
formation of hydroxide complexes of Cd(II) could lead to an increase in adsorption

efficiency. Magnetic biochar from agricultural biomass was applied to remove lead

and cadmium from wastewaters under different pH values. At lower pH values, the

cation concentration was high and the binding sites on surface were positively

charged, therefore Pb(II) and Cd(II) cations were repulsed, resulting in low removal

rate of metal ions. By increasing the pH of solution, the intensity of negative charge

on the surface of magnetic biochar was increased and the metal removal was

enhanced (Yap et al., 2017). The study on removal of phosphates from aqueous

solutions by magnetic zirconia-iron oxide nanoparticles showed that the phosphate

adsorption efficiency was decreased from 99.75 % to 41.06 % with the pH of solution

increasing from 1.5 to 10. This is probably due to the competition between phosphate

ions and the hydroxyl on the surface of adsorbent (Zhang et al., 2017).

On the other hand, the research on the effect of solution pH on As(V) adsorption

over pine biochar showed that the adsorption capacity of As(V) decreased with

solution pH. When pH of the solution was between 3 and 9, H2AsO4- and HAsO42-

were main negative oxygenated anions, therefore positively charged metal oxide

adsorption was at predominant position (Cho et al., 2017). Li et al. studied the

recovery of phosphate from aqueous solution by magnesium oxide decorated

magnetic biochar (Li et al., 2016b). It was found that the Fe and Mg oxides in

solutions could be protonated into FeOH+ and MgOH+ under lower initial pH,

resulting in an increase of adsorption capacity of magnetic biochar. The FeOH+ and

MgOH+ in solution might be the active centers for electrostatic adsorption of HPO42-

11
or H2PO4-. The positive charge surfaces of magnetic biochar became negatively

charged due to deprotonation by increasing the pH of solution, resulting in

electrostatic repulsion between the negatively charged surface of magnetic biochar

and the phosphate anion. Therefore, adsorption of phosphorus was eventually

decreased (Li et al., 2016b).

The study on the removal of Cd(II) and Pb(II) at different pH of solution by

magnetic biomaterial showed that the removal rates of Cd(II) and Pb(II) dramatically

increased with the pH of solution ( within the lower pH range). When the pH of

solution was 4.0, the removal rates of Cd(II) and Pb(II) reached a constant value of

99.75 % and 95.72 %, respectively. However, as the solution pH further increased,

removal rate of these two metal ions remained unchanged (Lalhmunsiama et al.,

2017). Wang et al. reported the influence of solution pH on norfloxacin (NOR)

adsorption by magnetic biochar. The results showed that the lowest adsorption of

NOR was obtained when the pH of solution was 2. The adsorption capacity increased

as the pH of solution increased from 4 to 7, and then tended to be stable after the pH

of solution exceeded 7 (Wang et al., 2017a). The increase of pH value was favorable

for the adsorption of NOR by magnetic biochar, which was probably due to that the

NOR exhibited diverse morphologies under different pH values.

3.1.4. Influence of adsorbent dosage on the removal of pollutants

The adsorption of Cd(II) ions under different doses of iron-modified biochar (5,

7.5 and 10 g/dm3) was investigated (Kolodynska et al., 2017). It was found that the

adsorption capacity of pollutants decreased with the increase of magnetic biochar

12
dosage. Through analyzing the adsorption of Cr(VI) by different amounts of

Na2SO3/FeSO4 modified peanut straw biochar, it was found that both the solution pH

and the removal rate of Cr(VI) increased with the increase of biochar dosage (Pan et

al., 2014). When the amount of magnetic biochar reached to 4 g/L and the pH of

solution was 7.1, the removal rate of Cr(VI) (1.5 mM) was 100 %. Meanwhile, by

increasing the amount of magnetic biochar, the adsorption of antibiotics decreased,

but the removal rate increased from 23.4 % to 99.1 %.

The adsorption efficiency was significant influenced by the dosage of adsorbent.

Under normal circumstances, the removal rate of pollutants increases with the

increase of magnetic biochar dosage, but unit adsorption capacity decreases with the

increase of magnetic biochar dosage. It is of great importance to optimize the dosage

of magnetic biochar for removal of water pollutants.

3.1.5. Effect of contact time on the removal of pollutants

Yap et al. evaluated the variation of cadmium concentration with time (Yap et al.,

2017). In the initial stage, it was observed that the adsorption rate sharply increased.

After a period of time (50-100 minutes), the adsorption rate slowed down and tended

to be stable. The removal of Cd(II) and Pb(II) ions from aqueous solutions by

synthetic mineral adsorbents was investigated. The sorption capacity of Cd(II) and

Pb(II) increased rapidly during the first 20 minutes due to the large surface area of the

adsorbent. Thereafter, due to saturation of the adsorption sites on the adsorbent

surface, the adsorb rate of Cd(II) and Pb(II) gradually slowed down and eventually

achieved equilibrium at the 30th minute. The formation of insoluble silicates on the

13
magnetic biochar prevented the adsorbate from entering into the internal sorption

layer (Chen et al., 2017a; Jung et al., 2017). The phosphate adsorption behavior of

magnesium ferrite/biochar magnetic composites in aqueous solution was investigated

(Jung et al., 2017; Peng et al., 2014). At the first 2 hours, phosphate adsorption

showed a rapid increase, and about 90 % of the initial phosphate concentration was

adsorbed at this stage. Then as the contact time increased to 10 hours, the adsorption

reached to equilibrium phase. This results can be due to: i) gradual saturation of the

available adsorption sites, ii) repulsive forces between phosphates, and iii) the

decrease of concentration gradient of phosphate in the bulk solution and the adsorbent

(Jung et al., 2017; Peng et al., 2014). However, through studying the removal

behavior of Cr(VI) from aqueous solution by Na2SO3/FeSO4 complexes, it was

observed that the remaining Cr(III) decreased with reaction time, and the optimum

reaction time for removal of Cr was 6 h. By increasing the reaction time, the pH of

solution increased (Pan et al., 2014).

Normally, the removal rate of pollutants by magnetic biochar increased rapidly at

the initial contact stage. After that, the removal rate of contaminants decreased due to

the saturation of adsorption sites, the formation of insoluble substance on the surface

of biochar, the repulsive forces between contaminants.

3.1.6. Effect of initial pollutant concentration on the removal of pollutants

The concentration of pollutant is also an important factor affecting the adsorption

capacity of magnetic biochar. Essandoh et al. studied the adsorption of metribuzin

from aqueous solutions using magnetic biochar under different initial pollutant

14
concentrations (Essandoh et al., 2017). It was found that the uptake of metribuzin

increased from 15.1 to 39.6 mg/g as the initial metribuzin concentration increased

from 40 to 100 mg/L by using magnetic switch grass biochar (MSGB) as adsorbent.

This demonstrated that MSGB provided a stronger driving force for adsorption of

metribuzin with high initial concentration. Moreover, the study on adsorption of

phosphate with different initial concentrations showed that high initial phosphate

concentration could enhance the phosphate adsorption by magnesia ferrite/Biochar

(Jung et al., 2017). This is probably attributed to the fact that the concurrent increase

of phosphate in liquid phase increased the contact opportunity between available

binding sites and phosphate on the surface of the magnesia ferrite/Biochar.

3.1.7. Effect of competitive anions on the removal of pollutants

Competitive ions have an important effect on the removal of pollutants, as these

ions can compete with pollutant ions for the adsorption sites of biochar.

Acid ions have a certain promoting or inhibiting effect on the adsorption of

heavy metals and organic matter. The study of the influence of competitive ions on

adsorption of arsenic by rice husk-derived magnetic biochar showed that the

competitive ions had an impact on the adsorption of arsenic (Cope et al., 2014).

Phosphate is one of the most common competitive ions, followed by silicate and then

sulfate. The study of influence of SO42- and NO3- on As(III) adsorption revealed that

the order of influence of competitive anions on As(III) absorption was PO43-> SO42->

NO3- (Lin et al., 2017). Another research showed that the binding attraction between

Cl- and As(III) was weaker than that between PO43- and As(III) and the influence of

15
competitive anions on As(III) removal followed the order: PO43-> HCO3-> Cl- (Baig et

al., 2014). For organic contaminants, competitive ions also have important impacts on

the adsorption and removal of organic pollutants. Wang et al. studied the adsorption

of acidic orange 7 (AO7) with different inorganic anions (Wang et al., 2017b). They

found that most of anions inhibited the removal of AO7, and the inhibition levels

were in the order of CO32->HCO3->H2PO4->SO42->NO3-. The effect of two halide

irons on the adsorption of AO7 was also studied. At low concentration of 1.85 mM,

Cl- and Br- increased the efficiency of oxidative degradation and slightly promoted the

removal of AO7. However, high concentration of these halide irons inhibited the

removal of AO7. Through investigating the removal of phosphates using nano-sized

magnetic zirconia-iron oxides, it can be seen that as common anions (Cl-, SO42- and

NO3-) increased from 0 to 150 mg/L, there was no obvious decrease of removal rate of

phosphate, indicating the three anions had no significant effect on the phosphate

adsorption (Zhang et al., 2017). However, the coexistence of HCO3- and phosphate

could inhibit the adsorption of phosphate, which was probably attributed to the strong

competition between HCO3- and phosphate for adsorption sites.

Salt ions and metal ions also have promoting or inhibiting effect on the

adsorption of pollutants. The influence of background electrolyte on the adsorption of

Cr(VI) by 0.01 mol/L of NaCl, Ca(NO3)2, CaCl2, Na3PO4 and Na2SO4 solutions was

investigated (Zhang et al., 2015b). The order of adsorption capacity was NaCl>

Ca(NO3)2> CaCl2> Na3PO4> Na2SO4. The study on the removal of Cr(VI) by

electrolytes shows that electrostatic force is a possible adsorption mechanism for the

16
removal of Cr(VI) by magnetic biochar. The impact of Na+, Mg2+ and Ca2+ ions on

Cd2+ and Pb2+ adsorption by magnetic biochar was studied (Chen et al., 2017b). The

results showed that even if the concentration of Na+, Mg2+ and Ca2+ increased to a

high level, no significant effect on the removal of Pb2+ was observed. However, the

presence of Na+, Mg2+ and Ca2+ had significant effects on the removal of Cd2+,

especially for Ca2+ (Chen et al., 2017b).

3.1.8. Effect of adsorption temperature on the removal of pollutants

Sun investigated the removal of crystal violet by the biochar coated with Fe3O4

under different temperatures (Sun et al., 2015). The adsorption capacity gradually

increased as the temperature increased from 293 to 313 K and the optimum adsorption

temperature was 313 K, which indicated that adsorption of crystal violet adsorption

by MBC was an endothermic process. Through analyzing the removal of fluorine

from groundwater using magnetic and non-magnetic corn stalk biochar as adsorbent,

it was found that the removal rate of fluoride by corn straw-derived biochar and

magnetic biochar gradually decreased as the adsorption temperature increased from

298 to 318 K (Mohan et al., 2014b). The metribuzin molecule absorption with

magnetic switchgrass biochar as adsorbent was carried out at 298, 308 and 318 K, it

was showed that the adsorption amount of metribuzin increased slightly with the

temperature increasing from 298 to 308 K while remained unchange within the

temperature range of 308 to 318 K (Essandoh et al., 2017).

The influence of adsorption temperature on the removal of pollutants in water by

different biochars is multilevel, which should be analyzed by case study.

17
3.2. Adsorption isotherm

Magnetic biochar as an adsorbent for removal of water contaminants has become

one of the major research focuses. In order to analyze the experimental data and the

adsorption equilibrium of heavy metals on magnetic biochar, various empirical

models have been introduced. The commonly used models include Freundlich,

Langmuir, Temkin equations and Langmuir-Freundlich models. The Langmuir model

assumes that monolayer adsorption takes place on homogeneous surfaces and there is

no interaction between adsorbed molecules. Freundlich models are often empirical

formulas for heterogeneous surfaces (Xue et al., 2012).

Han et al. studied the Cr(II) adsorption isotherms at different peak temperature

from 723 to 923 K. According to the resulting correlation coefficients, Langmuir

model was much more suitable for describing the adsorption isotherms of Cr(II) than

the Freundlich model (Han et al., 2016). Yap et al. used Langmuir, Freundlich and

Temkin equations to fit the adsorption data of Cd(II) and Pb(II). The corresponding

correlation coefficients (R2) indicated that the Langmuir equation presented the best

fitting performance (Yap et al., 2017). As shown in Table 2, it can be concluded that

Langmuir model is more appropriate to describe the equilibrium adsorption of heavy

metals by magnetic biochar in most cases. However, some studies showed that the

dynamic data of heavy metal adsorption by magnetic biochar fitted better to

Freundlich isotherm model than Langmuir isotherm model (Agrafioti et al., 2014;

Lalhmunsiama et al., 2017). Moreover, some studies showed that the dynamic data of

heavy metal adsorption by magnetic biochar fitted both Freundlich isotherm model

18
and Langmuir isotherm model (Mohan et al., 2014a; Mubarak et al., 2013; Wang et

al., 2015b; Wang et al., 2015c). Through investigating As(V) and Cr(VI) adsorption

by magnetic biochar derived from rice husk and organic fraction of municipal solid

wastes, it was found that the adsorption behavior of As(V) and Cr(VI) fitted better to

Freundlich equation (Agrafioti et al., 2014). Lalhmunsiama et al. investigated the

removal of Cd(II) and Pb(II) by the magnetic biomaterial which was prepared through

impregnating iron oxide nanoparticles with the Chlorella vulgaris (Lalhmunsiama et

al., 2017), and found that the sorption isotherms of Cd(II) and Pb(II) were better fitted

to Freundlich equation than Langmuir equation (Lalhmunsiama et al., 2017). Lin et al.

investigated the removal of As from aqueous solution by a novel Fe-Mn modified

magnetic biochar composite (Lin et al., 2017). The result showed that the adsorption

isotherm of As(III) was well suitable for both Freundlich equation and Langmuir

equation (Lin et al., 2017).

19
Table 2 Preparation and adsorption characteristics of heavy metals in water by different magnetic biochars

Heavy metal Feedstock Reagent Isotherm model Kinetic model Reference

U(VI) Rice husk Siderite Langmuir Pseudo-second-order model (Li et al.,

2019c)

Cu Rice straw ZnCl2 and FeCl3·6H2O Langmuir Pseudo-second-order model (Yin et al.,

2018)

Cr(VI) Peanut hull Iron chloride and Langmuir Pseudo-second-order model (Cai et al.,

hexamethylenediamine 2019)

Pb(II) Oil-tea and camellia shells FeCl2, Fe(NO3)3 and Langmuir Pseudo-second-order model (Jia et al.,

Mg(NO3)2 2019)

Cr(VI) Enteromorpha prolifera FeCl3 Langmuir Elovich model (Chen et al.,

2018a)

Cr(VI) Sugarcane bagasse, rice straw, Steel pickling waste liquo Freundlich Pseudo-second-order model (Yi et al.,

20
 peanut shells and herb residue 2019)

Sb(V) Phragmites australis LaCl3, FeCl3·6H2O, and Langmuir Pseudo-second-order model (Wang et

FeCl2·4H2O al., 2018)

Cr(VI) Phoenix tree leaves Fe3O4@SiO2 -NH2 Langmuir Pseudo-second-order model (Shi et al.,

2018)

Pb(II) Fresh paulownia tree litter CeO2-MoS2 hybrid Langmuir Pseudo-second-order model (Li et al.,

2019d)

Pb(II) Sludge Persulfate-ZVI Langmuir Pseudo-second-order model (Chen et al.,

2018b)

U(VI) Hydrophyte biomass Fe3O4 Langmuir - (Hu et al.,

2018)

Cd(II) Palm fiber Fe3O4 Langmuir Pseudo-second-order model (Zhou et al.,

2018b)

21
Cd(II) Rice straw Fe3O4 and CaCO3 Langmuir - (Wu et al.,

2018)

Cr(VI) Melia azedarach wood Fe3O4 Langmuir Pseudo-second-order model (Zhang et

al., 2018)

Cr(VI) Loofah sponges FeCl3 Freundlich Pseudo-second-order model (Xiao et al.,

2019)

Sb(V) Phragmites australis CeCl3·7H2O, FeCl3·6H2O Langmuir Pseudo-second-order model (Wang et

and FeCl2·4H2O al., 2019b)

Pb(II) Palm fiber Fe3O4 - The sips model and (Zhou et al.,

pseudo-second-order model 2018a)

As Pinewood Hematite Langmuir - (Wang et

al., 2015d)

As(V) Pinewood Fe and Mn ions Langmuir and Freundlich Second order and Elovich models (Wang et

22
 al., 2015c)

As(V) Chestnut shell and magnetic gelatin Fe3+/Fe2+ Langmuir Pseudo-second-order model (Zhou et al.,

2017)

As(III), As (V) Kans grass straw Fe3+/Fe2+ Langmuir Pseudo second-order model (Baig et al.,

2014)

As(V) Water hyacinth Fe3+/Fe2+ - - (Zhang et

al., 2016)

As(V) Pinewood Ni/Mn Langmuir and Freundlich Pseudo second-order model (Wang et

al., 2016b)

As(V) Chitosan Fe3+/Fe2+ Langmuir Pseudo second-order model (Liu et al.,

2017)

As(V) Coffee ground FeCl3 Langmuir Pseudo second-order model (Cho et al.,

2017)

23
 Cd Coconut shells FeCl3·6H2O Langmuir Pseudo -second-order model (Yap et al.,

2017)

Cd Rape straw FeCl3 Langmuir Pseudo-second-order model (Li et al.,

2017a)

Cd Oak wood Fe3+/Fe2+ Langmuir-Freundlich Pseudo- second-order model (Mohan et

al., 2014a)

Cd Rice straw Fe3+/Fe2+ Langmuir Pseudo -second-order model (Tan et al.,

2016)

Cr(VI) Chitosan Fe2O3 Langmuir Pseudo second-order model (Zhang et

al., 2015b)

Cr(VI) Herb-residue Fe3+/Fe2+ Langmuir Pseudo second-order model (Shang et

al., 2016)

Cr(VI) Pine sawdust Fe3O4 Langmuir Pseudo second-order model (Li et al.,

24
 2019b)

Cr(VI) Cotton stalk FeSO 4·7H2O, FeCl3· 6H2O Sips Pseudo second-order model (Ma et al.,

2019)

Cr(VI) Rice husk Fe0 /Fe3+ Freundlich - (Agrafioti et

al., 2014)

Pb Coconut shells FeCl3·6H2O Langmuir Pseudo -second-order model (Yap et al.,

2017)

Pb Sewage Sludge Fe3+/Fe2+ Langmuir Pseudo-second-order model (Ifthikar et

al., 2017)

Pb (II) Cane Fe3+/Fe2+ Langmuir Pseudo-second-order model (Mohan et

al., 2015)

Pb (II) Rice husk Ferric Acetylacetonate and Langmuir Pseudo-first-order model (Yan et al.,

zinc chloride 2015)

25
 Zn(II) Multiwall carbon nanotubes FeCl3 Langmuir and Freundlich Pseudo-second-order model (Mubarak et

al., 2013)

Cd(II), Co(II), Agricultural wastes Zero-valent iron Langmuir Pseudo-second-order model (Kolodyns

Zn(II) and Pb(II) ka et al.,

2017)

Cd and Pb Chlorella vulgaris FeSO 4·7H2O, FeCl3· 6H2O Freundlich Pseudo-second -order model (Lalhmunsi

ama et al.,

2017)

Cd and Pb Chlorella vulgaris FeSO 4·7H2O, FeCl3· 6H2O Freundlich Pseudo-second -order model (Lalhmunsi

ama et al.,

2017)

Pb and Cd Sulfonated magnetic nanoparticle Fe3O4 Langmuir Pseudo-second-order model (Chen et al.,

2017b)

26
As and Sb Sludge Fe3O4 Langmuir Pseudo-second-order model (Wang et

al., 2016a)

As and Pb Pine wood MnCl2·H2O Langmuir and Freundlich Elovich kinetic model (As(V)) (Wang et

and the first and second order al., 2015b)

model (Pb(II))

Ag(I) Apple pomace Fe3+/Fe2+ - Pseudo-second-order model (Zhang et

al., 2019)

27
 Magnetic biochar is also effective in adsorption of organic pollutants. In the past

few years, many researchers have found that magnetic biochar can act as an efficient

adsorbent for removal of organic pollutants in water, such as pesticides, antibiotics,

pharmaceuticals and so on. The adsorption properties of organic pollutants by

magnetic biochars are shown in Table 3.

The thermodynamic mechanism of adsorption of organic compounds is

complicated. As shown in Table 3, most of the adsorption isotherms of organic

contaminants by magnetic biochars fit to Langmuir or Freundlich isotherm model.

Through investigating the removal of metribuzin from water by using switch grass

derived magnetic biochar, it was found that Langmuir model was more suitable to

describe the adsorption of metribuzin by magnetic biochars (Essandoh et al., 2017).

Similarly, the studies of crystal violet adsorption (Sun et al., 2015), antibiotic

adsorption (Kong et al., 2017), norfloxacin adsorption (Wang et al., 2017a),

Carbamazepine (CBZ) and tetracycline (TC) adsorption (Shan et al., 2016) reached

the same results. However, Li et al. suggested that Freundlich model fitted the data

better than Langmuir model for the adsorption of aromatic contaminants by using

magnetic biochar derived from pyrolysis oil distillation residue (Li et al., 2017b).

Nevertheless, Karunanayake et al. found that the adsorption isotherms of salicylic

acid, 4-nitroaniline, benzoic acid and phthalic acid from wastewater by using

magnetized fast pyrolysis biochar fitted the data to Sips, Redlich-Peterson and Toth

models better than Langmuir and Freundlich models (Karunanayake et al., 2017).

In the study of phosphate adsorption by corn cob biochar and wood waste

28
biochar, the adsorption data of PO43− better fitted to DKR model. In contrast, the

adsorption parameters using wood chip-derived biochar, magnetic corn cob biochar,

magnetic wood waste biochar and magnetic wood chip-derived biochar as adsorbents

fitted to Langmuir and Freundlich models (Michalekova-Richveisova et al., 2017).

29
Table 3 Preparation and adsorption parameters of organic contaminants and phosphate in water by different magnetic biochars

Organic contaminants Feedstock Reagent Isotherm model Kinetic model Reference

4-nonylphenol Bamboo Fe3O4 Langmuir-Hinshelwood Pseudo-first-order model (Dong et

al., 2019)

Bisphenol A and Bamboo Fe2O3, 25% ZnO Langmuir Pseudo-second-order model (Heo et

sulfamethoxazole and 35% CuO al., 2019)

Florfenicol Reed stalk Fe2(SO4)3 Langmuir Pseudo-second-order model (Zhao and

Lang,

2018)

Tetracycline Municipal sludge Alkali-acid Langmuir-Freundlich Pseudo-second-order model (Zhou et

al., 2019)

Daptomycin Wood Fe3O4 Freundlich - (Ai et al.,

2019)

30
 ciprofloxacin Camphor leaves ZnO Langmuir Pseudo-second-order model (Hu et al.,

2019)

Tetracycline and fluorescent dye Chicken bone KMnO4 Freundlich - (Oladipo

and

Ifebajo,

2018)

17β-estradiol Bagasse FeCl3·6H2O and Langmuir Pseudo-second-order model (Dong et

FeSO4·7H2O al., 2018)

Tetracycline Sewage sludge NaOH, HNO3 and Freundlich Evolich model (Tang et

CH3COOH al., 2018)

Acid orange 7 Marine macroalgae Fe3O4 Langmuir and Freundlich - (Jung et

al., 2016)

Aniline and nitrobenzene Douglas fir FeCl3 Langmuir and Freundlich - (Dewage

31
 et al.,

2019)

Aromatic contaminants Oil distillation residue Fe(NO3)3 Freundlich - (Chen et

al., 2017c)

Antibiotic Herbal medicine waste FeCl3·6H2O and Langmuir Pseudo second-order model (Kong et

FeSO4·7H2O al., 2017)

Crystal violet Corn stalks Fe3O4 Langmuir Pseudo second-order model (Sun et

al.,

2015)

Carbamazepine tetracycline Coconut, pinenut and Fe, Fe2O3 or Fe3O4 Langmuir - (Shan et

walnut shells al., 2016)

Metribuzin Switchgrass Fe3+/Fe2+ Langmuir Pseudo second-order model (Essandoh

et al.,

32
 2017)

Norfloxacin Corn stalks, reed stalks, FeCl3 Langmuir Pseudo second-order model (Wang et

and willow branches al., 2017a)

Salicylic acid, 4-nitroaniline, Waste Douglas fir Fe3+/ Fe2+ Sips, Redlich Peterson and - (Karunana

benzoic acid and phthalic acid Toth models yake et al.,

2017)

sulfamethoxazole pine sawdust FeCl2 Redlich-Peterson isotherm Pseudo-second order model or the (Reguyal

Feundlich pseudo-first order model et al.,

2017)

Tetracycline Waste hydrochar FeCl3 Freundlich Pseudo second-order model (Zhu et

al., 2014)

Phosphate Corn cob, garden wood Fe(NO3)3 Langmuir and Freundlich Pseudo-nth order model (Michale

waste, wood chip models kova-Ric

33
 hveisova

et al.,

2017)

Phosphate Zirconium-iron oxide Fe/Zr Freundlich Pseudo-second order model (Zhang et

nanoparticles al., 2017)

Phosphate Water hyacinth Fe Langmuir-Freundlich Pseudo second-order model (Cai et al.,

2017)

Phosphate sugarcane harvest residue Fe Langmuir - (Li et al.,

2016b)

Phosphate Undaria pinnatifida roots FeCl3·6H2O and - Pseudo-second-order model (Jung et

MgCl2·4H2O al., 2017)

Phosphate Pineapple peel La(OH)3 Langmuir Pseudo-second-order model (Liao et

al., 2018)

34
Phosphate Pristine CeCl3·7H2O or Freundlich Pseudo-second-order model (Wang et

LaCl3 with al., 2019a)

FeCl3·6H2O and

FeCl2·4H2O

35
3.3. Adsorption kinetics

The studies of adsorption kinetics of magnetic biochar provides references for

investigating the chemical adsorption and heterogeneous catalytic reaction mechanism.

The research on adsorption kinetics of magnetic biochar is of importance to the

removal process of contaminants. Three kinds of kinetic models are normally used to

investigate the contaminants adsorption by magnetic biochars, including

pseudo-first-order kinetic model, pseudo-second-order kinetic model and Elovich

model. The best-fit kinetic models to analyze the removal of organic and inorganic

contaminants by magnetic biochars are summarized in Table 2 and Table 3.

Li et al. used pseudo-first-order, pseudo-second-order and intra-particle models

to study the adsorption mechanism of Cd(II) by rape straw-derived magnetic biochar

(Li et al., 2017a). The kinetic data fitted well to the pseudo-second-order model, and

cation-π bonding and cation exchange were the main mechanisms responsible for the

increase in adsorption capacities of MnOx-loaded biochar. Cho et al. found the same

result via studying of the adsorption mechanism of As(V) onto magnetic biochars

(Cho et al., 2017). In the study of the kinetic and adsorptive characterization of Pb(II)

by magnetic biochar, it was found that the adsorption kinetic process of Pb(II) fitted

well to pseudo-second-order model (Chen et al., 2018b). Moreover, some other

studies showed that the adsorption kinetic process of metals by magnetic biochars can

be better described by the pseudo-first-order kinetic model. Yan et al. used Magnetic

biochar/ZnS composites to remove Pb(II), and the results showed that the adsorption

kinetics of Pb(II) fitted better to pseudo-first-order kinetics model than second-order

36
kinetic model (Yan et al., 2015).

Most adsorption kinetics of organic contaminants on magnetic biochars can be

described by pseudo-second-order model. The adsorption kinetics of tetracycline on

magnetic porous carbon derived from waste hydrochar was reported well fitted to the

pseudo-second-order model (Zhu et al., 2014). Reguyal et al. reported the kinetic and

adsorptive characterization of sulfamethoxazole(SMX) on magnetic biochar (Reguyal

et al., 2017). The result showed that the kinetic data better fitted to the pseudo-second

order model at low concentrations of SMX (1 to 5.1 mg/L), while the pseudo-first

order model was more suitable to describe the kinetic data at high SMX concentration

of 20.5 mg/L. As reported by researchers, the adsorption kinetics of phosphate onto

magnetic biochar better fitted to pseudo-second-order model (Cai et al., 2017; Jung et

al., 2017; Michalekova-Richveisova et al., 2017; Zhang et al., 2017).

In general, most of the adsorption kinetics of contaminants on magnetic biochars

better fit to the pseudo-second-order model.

4. Adsorption mechanism

Understanding the adsorption mechanism of magnetic biochar is important for

rational utilization of magnetic biochar in water treatment. Fig. 2 shows the

adsorption mechanisms of contaminants on magnetic biochar, including surface

complexation, electrostatic attraction, chemical precipitation, coordination reaction,

ion exchange, hydrogen bond and so on. The adsorption mechanisms vary with

pollutants and is influenced by the pore structure, functional groups and chemical

bonds on the surface of the magnetic biochar.

37
 There is a correlation between the adsorption mechanisms of pollutants and the

nature of magnetic biochar. By reviewing existing literatures, it can be concluded that

electrostatic attraction, ion exchange, surface complexation and O-containing groups

are the primary mechanisms for adsorption of heavy metal pollutants on magnetic

biochars.
M- H2 +
M-
M M
ph<phpzc
O H2+ Anionic metal attraction
M- H2 +
O C O
O O
M R
O
R
O
Ma
C
M

M
C M+
Ma
M R O R O
O O- O C
O O-
M+
O-
M
M +
ph<phpzc M
Cationic metal attraction

Ion
(a) Ion exchange (b) Electrostatic attraction

M
H

O
H M
M
H
O M+
R O
C Ma 

Ma C
O R H 
O M
M H
O M+
H
M

(c) Surface complexation (d) Co-precipitation

M
H
Surface complexation
H
Hydrogen bonds O M π-π H O
interactions O
C
R
C
H O H
O

H O O
O M H
H C
C
P-P M C O
O H
interactions
O O H H M

(e) Chemical bond (f) Oxygen-containing functional groups

38
 Reduction

M Mr
Ma Physical
adsorption

Mr M
Ma
Pore-filling
Reduction
(g) Reduction (h) Others

 Exchangeable metal ions (Ca2+, Mg2+, K+, Na+)

M Metal ions
Ma Metals attached on magnetic biochar
 Ions in magnetic biochar such as phosphate and carbonate
Mr Reduced form of metal ions

Fig. 2. Adsorption mechanisms of metal ions in water by magnetic biochars

4. 1. Ion exchange

In order to extracting or removing certain ions from the solution, ion exchange is

normally carried out. This unit operation belongs to the mass transfer separation

process. Ion exchange is a reversible equivalent exchange reaction, and the adsorption

mechanism is shown in Fig.3(a).

Lukáš Trakal studied the adsorption mechanism of Pb and Cd on magnetic

biochar (Trakal et al., 2016). The FTIR spectra showed that the association between

Pb(II) and CO32- existed in/on all magnetic biochars. The peak at 1427 or 1438 cm-1

for CO32- was shift to 1383 cm-1 after metal adsorption (especially after Pb(II)

sorption). Based on the XPS analysis, it could be deduced that ion exchange was a

significant metal adsorption mechanism. Meanwhile, XRD spectra showed significant

shift of peaks for carboxyl groups (1558-1566 cm-1 and 1695-1701 cm-1) after Cd and

Pb loading. This demonstrated that metal chelates was formed on the surface of

39
magnetic biochars during the adsorption process (Trakal et al., 2016). However,

previous studies showed that chelation was not the main metal adsorption mechanism

of biochar. This difference might be due to the magnetic modification of biochar,

which altered the chemical properties such as pH and PZC values of the magnetic

biochars (Trakal et al., 2014).

On the other hand, Zuo et al. studied the adsorption mechanism of Cd(II) from

aqueous solution using CaCO3 nanoparticle modified sewage sludge biochar (Zuo et

al., 2017). The results showed that the intensity of the corresponding band appearing

at 1427 and 879 cm-1 decreased significantly after the adsorption of Cd(II) by calcium

carbonate modified sludge biochar. The decrease of both peaks was due to the surface

exchange of ions or metal(hydro)carbonates. Chen et al. studied the adsorption

mechanism of cadmium and lead ions from water using sulfonated magnetic

nanoparticle adsorbents (Chen et al., 2017b). The FTIR and XPS data demonstrated

that cation exchange was an important approach for removal of ions on sulfonated

magnetic nanoparticle. The sulfo-binding sites on the surface of magnetic biochar

allowed the formation of heavy metal ion complexes which significantly improve

adsorption capacity of magnetic biochar.

4.2. Electrostatic interaction

Electrostatic interaction, including electrostatic attraction and electrostatic

repulsion, is a necessary process to form chemical bonds and ionic bonds. The

mechanism of electrostatic interaction is shown in Fig.3(b).

By investigating the removal of As(V) and Cr(VI) from aqueous solution using

40
modified biochar as adsorbents, it was found that the main mechanism for removal of

As(V) and Cr(VI) might be the electrostatic interaction between the modified biochars

and the adsorbate (Agrafioti et al., 2014). The XRD analysis of adsorbed biochar

samples showed that no new peaks were formed, indicating precipitation was not the

dominating mechanism for removal of As(V) by pine magnetic biochar (Wang et al.,

2015d). The interaction between HAsO42- and the positively charged functional

groups on the surface of hematite modified biochar might occur through electrostatic

attractions. By investigating the adsorption mechanism of As(V) on magnetic

chitosan/biochar composite (MCB), it could be known that after adsorption, the molar

ratio of N+ on MCB increased from 13.3 % to 16.2 %, the molar ratio of -NH- on

MCB decreased from 64.7 % to 61.4 %, and that of -NH2 on MCB remained

unchanged (Liu et al., 2017). This demonstrated that the N+ might play a vital role in

removal of As(V) by absorbing H2AsO4- or HAsO42- through electrostatic attraction.

Other studies on the adsorption of As(III, V) from aqueous solution using magnetic

Kans grass biochar showed that the electrostatic attraction was the main mechanism

for the adsorption of As(III, V) by magnetic biochar, and the electrostatic attraction of

As(III, V) on magnetic biochar might lead to the formation of specific inner-sphere

complexation with hydroxyl groups. However, other adsorption mechanisms, such as

surface complexation, chemical adsorption and ion exchange, should not be ignored

during the adsorption process (Baig et al., 2014).

The main adsorption mechanisms of As(V) on Ni/Mn-LDHs precipitated pristine

biochars (NMMB) were anion exchange and surface complexation, while the As(V)

41
adsorption was mainly attributed to surface complexation by Ni/Mn oxide modified

pinewood material (NMMF) (Wang et al., 2016b). The formation of surface complex

was supported by altering the binding energies of O1s for Ni/Mn-LDHs precipitated

biochar. HAsO42- might be adsorbed by Cl- and NO3- existing in the Ni/Mn-LDHs

precipitated biochar. No change of O1s binding energy was observed for

Ni/Mn-LDHs precipitated biochar before and after adsorption with NMMF(Wang et

al., 2016b).

Khare et al. investigated the adsorption mechanism of Pb(II) on magnetic sewage

sludge biochar (MSSBC) (Ifthikar et al., 2017). The adsorption mechanisms of Pb(II)

on MSSBC were mainly physical adsorption and chemisorption. From the N2-sorption

and SEM images, it could be seen that the high surface area and porous structure of

MSSBC did make Pb(II) easily access to the surface of MSSBC and generate physical

adsorption (Ifthikar et al., 2017). The influence of pH and zeta potential measurement

confirmed that electrostatic attraction occurred between MSSBC and Pb(II), and the

removal of heavy metal ions by MSSBC was mainly dependent on chemical

adsorption rather than physical adsorption (Ifthikar et al., 2017).

4.3. Surface complexation

Complexing is a process during which electron donors and electron acceptors

interact with each other to form various complexes. Electron donors are providers of

electronic pairs, while acceptors are metal ions or organic compounds. The process

for molecular or ionic and metal ions to combine with each other to form a very stable

new ion is called complexation reaction or coordination reaction, and the adsorption

42
mechanism is shown in Fig.3(c).

Wang et al. investigated the adsorption mechanism of arsenate from aqueous

solutions by using biochar supported zero-valent iron nanocomposite (Wang et al.,

2017c). A 100 % removal efficiency was achieved in a completely mixed reactor,

with an initial As(V) concentration of 2.1 mg/L. Surface complexation might be the

dominant mechanism for removal of As(V), although reduction reactions might be

involved. Cai et al. investigated the adsorption mechanism of phosphate over water

hyacinth-derived magnetic biochar. The results showed that the adsorption of P on

MW450 was mainly based on ligand exchange and surface complexation with

hydroxyl groups (Cai et al., 2017).

4.4. O-containing functional groups combination

Combination mainly occurs between pollutants and functional groups of

magnetic biochar. Therefore, functional groups play a key role in O-containing

functional groups combination to removal contaminants from water. The adsorption

mechanism is shown in Fig.4(f).

Song et al. studied the synthesis, characterization and adsorption of Cu(II) from

aqueous solution by MnOx-Loaded biochars (Song et al., 2014) . The adsorption

capacity of Cu(II) over MnOx-loaded precursors was mainly dependent on the

formation of MnOx and O-containing groups on surface. In addition, other

mechanisms such as cation exchange and cation p bond might be also involved in

Cu2+ adsorption.

In the investigation of adsorption mechanisms of As(V), it was found that the

43
factors influencing the adsorption of As(V) mainly included the shape of As(V) and

the charge on the surface of magnetic gelatin-modified biochar (Chowdhury and

Yanful, 2010; Tuutijärvi et al., 2009). Harikishore studied the removal of mercury by

pine bark-derived magnetic biochar (Harikishore Kumar Reddy and Lee, 2014).

According to the FTIR spectroscopic data, it was observed that the major functional

group present on the magnetic biochar composite was hydroxyl. After adsorption of

metal ion, the peak of hydroxyl functional group was found significantly changed.

This indicated that metal ions might coordinate with the surface hydroxyl groups of

the magnetic biochar composite.

Magnetic sulfur dioxide from spent marine algal biomass showed high selectivity

of copper. This excellent performance in removal of heavy metal might be attributed

to the presence of various oxygen-containing functional groups, such as -COOH and

-OH, which can serve as the potential adsorption sites for heavy metals on magnetic

biochars (Son et al., 2017). Hu et al. investigated the adsorption mechanism of As(V)

by magnetic gelatin-modified biochar (Hu et al., 2015). When pH=4, As(V) was

mainly present in the form of HAsO42- and part of the functional groups in magnetic

biochar were protonated, thus the magnetic biochar was positively charged. The

differences in IR spectra before and after adsorption could be observed from the

newly appeared peaks at 910 cm-1 and 813 cm-1. The ion particles and surface

functional groups in magnetic gelation-modified biochar could further improve the

adsorption capacity of As(V) in aqueous solution (Zhou et al., 2017). Yang et al.

investigated the mechanism of simultaneous deactivation and the removal of mercury

44
by sawdust magnetic biochar (Yang et al., 2016). Two types of active

adsorption/oxidation sites for novel magnetic biochars were proposed. For removing

Hg0, Fe3O4 provided Fe3+(t) coordination and lattice oxygen. The functional group of

C=O acted as electron acceptors to promote electron transfer during the Hg0 oxidation

reaction.

The study by Pan showed that the adsorption mechanism of Cr(III) was mainly

due to formation of surface complexes with functional groups of biochar (Pan et al.,

2014). Agrafioti et al. found that metal precipitation and electrostatic interactions

were possibly the main mechanisms accounting for the removal of As(V) and Cr(VI)

by using the Ca and Fe modified biochars as adsorbent (Agrafioti et al., 2014).

According to the study on the mechanism for the removal of arsenic, it was found that

oxidation of Mn(III) and oxygen-containing functional groups of Fe/Mn modified

biochar promoted the conversion from As(III) to As(V) in aqueous solution, and

chemisorption was considered as the main mechanism for the adsorption of arsenic on

the Fe/Mn modified biochar (Lin et al., 2017).

4.5. Co-precipitation

Co-precipitation is a process to make some coexisting soluble substances

precipitate together. The process of co-precipitation involves surface adsorption,

mixed crystal, embedded and so on. The adsorption mechanism of co-precipitation is

shown in Fig.3(d).

The adsorption of arsenate using magnetic Fe-Mn biochar composites prepared

by direct pyrolysis of Fe and Mn ion pretreated pinewood biomass (FMM) or

45
co-precipitation of Fe and Mn ions onto pinewood biochar (FMB) was studied (Wang

et al., 2015c). It was found that the maximal As(V) adsorption was obtained when

FMB concentration was 3.44 g/kg, and the pH of solution played a role in controlling

the adsorption of arsenate onto FMB. The pHpzc of both FMM and FMB was greater

than 7.5. Co-precipitation is an efficient method to prepare magnetic Fe-Mn biochar

for removal of As(V) from aqueous solution.

4.6. Chemical bond adsorption

Chemical bond adsorption involves a strong interaction between two or more

adjacent atoms (or ions) in a molecule or a crystal. The adsorption mechanism is

shown in Fig.3(g).

According to the study on the removal of arsenate by magnetite-modified water

hyacinth biochar, the adsorption mechanism of As(V) was mainly to exchange As(V)

with H bond on the hydroxylated surface of Fe3O4 (Zhang et al., 2016). XPS analysis

further demonstrated that the main existing form of arsenic adsorbed on magnetic

biochar was As(V). In the study of Pb(II) removal by MnOx-loaded biochar, it was

found that adsorption mechanism was not limited to the participation of nano-sized

manganese oxide supported particles and available surface oxygen-containing

functional groups (Faheem et al., 2016), but vacancy defects and π-π* transitions also

influenced the adsorption process. Li et al. studied the main adsorption mechanism of

aromatic pollutants on magnetic biochar (Li et al., 2017b). The high surface area and

pore volume of magnetic biochar generally promoted the adsorption of anisole and

phenol. The main mechanism for the adsorption of guaiacol on magnetic biochar was

46
the π-π electron donor-acceptor (EDA) interaction, and the graphitic layers of the

magnetic biochar was considered as a π-electron donor (Li et al., 2016a). Therefore,

the interaction between guaiacol and magnetic biochar could be enhanced by

increasing graphite layer content. It was reported that, during the adsorption of

tetracycline onto magnetic carbon composites, the adsorption of tetracycline was

mainly attributed to the H bond and π-π interaction (Rattanachueskul et al., 2017).

4.7. Reduction

The mechanism of reduction adsorption is shown in Fig.3(e). Through the

systematic analysis of Pb(II) removal mechanisms, it was found that the reduction

mechanism might play a vital role in removal of Pb(II) by sludge magnetic biochar

(Chen et al., 2018b). Another research also showed that ferric chloride (FeCl3)

increased the porosity of magnetic carbon composites (MCs), which was mainly due

to the strong reduction between amorphous carbon and iron oxide (g-Fe2O3 and Fe3O4)

(Zhu et al., 2016).

5. Degradation of contaminants over magnetic biochar

Due to the high specific surface area and porous structure, magnetic biochar can

also be used as activator of some degradation catalysts. Rong et al. used the magnetic

biochar derived from banana peels as a persulfate activator for bisphenol A

degradation (Rong et al., 2019). It was found that the encapsulated γ-Fe2O3

nanoparticles enhanced the catalytic ability of persulfate activator and bisphenol (20

mg/L) was completely removed within 20 min by the magnetic biochar (Rong et al.,

2019). During the degradation process of bisphenol, the radical oxidation mechanism

47
played a dominant role. Li et al. investigated the hydrogen peroxide activation of

Fe-Mn binary oxides modified biochar for the degradation of naphthalene in water (Li

et al., 2019a). The degradation rate of naphthalene reached 75.8 % after 148 min by

using Fe-Mn binary oxides modified biochar. The results showed that the synergistic

effect of biochar and Fe-Mn binary oxides was important to the enhancement of

naphthalene degradation efficiency. Lai et al. fabricated a novel magnetic

MnFe2O4/biochar and investigated the heterogeneous photo-Fenton degradation

activity of tetracycline (Lai et al., 2019). Biochar played a role in decreasing the

aggregation of MnFe2O4. Higher degradation rate of tetracycline was obtained by

using MnFe2O4/biochar composite than using pure MnFe2O4.

6. Future prospects

More efforts should be carried out to study the removal of contaminants by

magnetic biochar. Based on the above discussions and investigations, the future

research on the preparation and application of magnetic biochar in water treatment can

be carried out from following aspects. 1) the impact of modifiers on the

physiochemical properties of magnetic biochar should be further studied in future; 2)

the removal of organic matters and phosphoric acid by magnetic biochar as well as the

adsorption and removal mechanism of organic matters need to be deeply explored; 3)

research on dealing with the toxic and harmful substances produced during the

production should be attached with high importance; 4) development of magnetic

biochar with catalytic degradation activity for organic contaminants in water is

another interesting research direction. It is believed that magnetic biochar will become

48
a research focus and gain greater development in the near future.

7. Conclusions

In this review, the application of various kinds of magnetic biochar for removing

contaminants in water is discussed, and the preparation methods for magnetic biochar

are summarized as well. The factors influencing the removal of water pollutants by

magnetic biochar are analyzed emphatically. The effects of pyrolysis temperature,

ratio of magnetic material injection and solution pH on the removal of water

pollutants are emphatically introduced. Compared with biochar, magnetic biochar has

a higher removal effect for water pollutants. The adsorption mechanisms of magnetic

biochar for removal of water pollutants are analyzed, including complexation, ion

exchange, electrostatic attraction, reduction, chemical precipitation and hydrogen

bonding. Besides, the potential of magnetic biochar as catalyst for degradation of

organic contaminants in water is investigated.

Acknowledgement

This work is financially supported by National Natural Science Foundation of

China through project (grant number 51602215 and 41502131), the Fundamental

Research Funds for the Central Universities (18CX02101A), the Guangdong

Provincial Key Laboratory of New and Renewable Energy Research and

Development (Y807s41001) and the National Science and Technology Major Project

(grant number 2016ZX05014-004-007).

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There are no conflicts of interest to declare.

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Graphical abstract

Magnetic Pyrolysis
material Other
contam
Animal waste Algae -inants

Magnetic
material Organic Heavy
Pyrolysis
contam-
inants
Adsorption metals

Biochar Magnetic biochar NP

Solid waste Straw

NP nutrients

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Highlights

 Influence factors on water pollutants adsorption by magnetic biochar

were analyzed

 Langmuir and Freundlich models are the main isotherms model for

pollutants in water

 Pseudo-second-order model are the main kinetic model for

contaminants in water

 The adsorption mechanisms of magnetic biochar in water are

analyzed

 Future development of magnetic biochar in pollutants removal was

prospected

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