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化学进展 2022, Vol. 34 Issue (4): 992-1010 DOI: 10.7536/PC210109 前一篇   

• 综述 •

基于生物炭的高级氧化技术降解水中有机污染物

吴飞1, 任伟1, 程成1, 王艳2, 林恒1,*(), 张晖1,*()   

  1. 1 武汉大学资源与环境科学学院 环境科学与工程系 生物质资源化学与环境生物技术湖北省重点实验室 武汉 430079
    2 安徽科技学院环境科学与工程系 凤阳 233100
  • 收稿日期:2021-01-14 修回日期:2021-06-07 出版日期:2022-04-24 发布日期:2021-07-29
  • 通讯作者: 林恒, 张晖
  • 基金资助:
    国家自然科学基金青年项目(21806125); 中国博士后科学基金面上项目(2016M602365); 中央高校基本科研业务费专项资金项目(武汉大学); 安徽省自然科学基金(1808085MB49)
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Biochar-Based Advanced Oxidation Processes for the Degradation of Organic Contaminants in Water

Fei Wu1, Wei Ren1, Cheng Cheng1, Yan Wang2, Heng Lin1(), Hui Zhang1()   

  1. 1 Key Laboratory of Hubei Biomass-Resource Chemistry and Environmental Biotechnology, Department of Environmental Science and Engineering, School of Resource and Environmental Sciences, Wuhan University,Wuhan 430079, China
    2 Department of Environmental Science and Engineering, Anhui Science and Technology University,Fengyang 233100, China
  • Received:2021-01-14 Revised:2021-06-07 Online:2022-04-24 Published:2021-07-29
  • Contact: Heng Lin, Hui Zhang
  • Supported by:
    National Natural Science Foundation of China(21806125); Postdoctoral Science Foundation of China(2016M602365); Fundamental Research Funds for Central Universities of China (awarded at Wuhan University); Natural Science Foundation of Anhui Province(1808085MB49)

碳基材料催化剂因具有良好的催化性能,同时可避免金属催化剂的重金属沥出造成的二次污染问题,常被应用于高级氧化领域。其中,以废弃生物质为原材料热解产生的生物炭,不仅具有催化潜力,还具有低成本和绿色环保等优势,被广泛用于活化过氧化氢、过一硫酸氢盐和过二硫酸盐等过氧化物降解水中有机污染物。本文介绍了生物炭的前体种类和制备方法、阐述了二者对生物炭活化能力的影响,总结了生物炭活化过氧化物的机理,分析了水质对降解污染物的影响,综述了生物炭的改性、循环使用及再生,指出了这一技术存在的问题并对后续研究进行了展望。

关键词： 生物炭, 高级氧化技术, 过氧化物, 自由基机理, 非自由基机理

Carbonaceous materials with superior catalytic activity, which could avoid drawbacks of heavy metal ion leaching for metal-based catalysts, are widely used in advanced oxidation processes (AOPs). Biochar, a carbon-rich material produced by pyrolysis of biomass under oxygen limited condition, is low-cost, widely available, and environmentally friendly. Biochar has been utilized to activate peroxides such as hydrogen peroxide, peroxymonosulfate and peroxydisulfate for the degradation of pollutants in water. In this paper, precursors and preparation methods of biochar as well as their influence on catalytic activity of biochar are discussed. The activation mechanisms of peroxides by biochar and the effects of water matrices on the degradation of pollutants are summarized. The progress in the modification of biochar is reviewed. The reusability of biochar is elucidated and the regeneration methods of biochar are provided. In the end, the problems and the prospects of the biochar-based AOPs are put forward.

Contents

1 Introduction

2 Biomass precursors

2.1 Lignocellulosic biomass precursors

2.2 Non-lignocellulosic biomass precursors

2.3 Effects of biomass precursors on catalytic performance of biochar

3 Preparation methods of biochar

4 Activating mechanism of peroxides by biochar

4.1 Radical mechanism

4.2 Non-radical mechanism

5 Effects of water matrices

5.1 Effect of pH

5.2 Effects of anions and NOM

6 Modification of biochar

6.1 Acid/base modification

6.2 Graphitizing modification

6.3 Doping modification

7 Reusability and regeneration of biochar

7.1 Change of physical properties

7.2 Change of chemical properties

7.3 Regeneration methods

8 Conclusion and prospection

Key words: biochar, advanced oxidation processes, peroxide, radical mechanism, non-radical mechanism
()
表1 不同前体的生物炭活化过氧化物降解水中有机污染物
Table 1 The degradation of organic pollutants by peroxides activated via biochar produced from different precursors
Biomass Oxidant Preparation Mechanism Active sites Reactive species Reaction condition Performance ref
Lignocellulose
biomass
Wheat; straw;
hardwood		 H2O2 Pyrolysis Radical Ash (Fe、Cu、Mn、Ni、Mo);
—OH;
—COOH		 ·OH (main), HO2·、·O2- Catalyst = 1 g/L
H2O2 = 5 mM
1-Methyl-1-cyclohexanecarboxylic acid = 500 mg/L
pH = 7		 99% mineralization of
1-Methyl-1-cyclohexanecarboxylic acid in 4 h		 52
Valorized
Olive Stones		 PDS Pyrolysis Radical N/A ·OH (main), ·SO4- both in solution and in the vicinity of BC surface Catalyst = 200 mg/L
PDS = 1000 mg/L
Sulfamethoxazole = 500 μg/L
Inherent pH		 70% degradation of
sulfamethoxazole in 75 min		 16
Corn stalk PDS Pyrolysis Nonradical Oxygen-containing functional groups ·OH, ·SO4- mainly on the
surface or boundary layer of BC		 Catalyst = 0.8 g/L
PDS/norfloxacin = 120/1
Norfloxacin = 10 mg/L
Initial pH = 6.5		 94% degradation of
norfloxacin in 300 min		 53
Sunflower PDS Pyrolysis Radical Defects ·OH, ·SO4- Catalyst = 5 g/L
PDS = 10 mM
p-Nitrophenol = 0.72 mM
Initial pH = 2.58
Temperature = 60 ℃		 86% degradation of
p-nitrophenol in 180 min		 54
Sawdust PDS Pyrolysis Radical —OH
π-π*		 Surface-bound ·OH, ·SO4-
(main);
·OH, ·SO4- in solution		 Catalyst = 0.5 g/L
PDS = 10 mM
Clofibric acid = 1 g/L
Initial pH = 4		 98% degradation of
clofibric acid in 60 min		 55
Wood PDS Pyrolysis Nonradical —OH
π-π*		 Surface-bounded ·OH, ·SO4-
(main)		 Catalyst = 0.5 g/L
PDS = 10 mM
AO7 = 20 mg/L
Initial pH = 6		 99% degradation of AO7 in 14 min 56
Rice straw PDS Pyrolysis Nonradical N/A Holes Catalyst = 0.6 g/L
PDS = 90 mg/L
Aniline = 10 mg/L
Initial pH = 3		 94% degradation of aniline in 80 min 57
Sawdust PDS Pyrolysis Radical
and
Nonradical		 N/A Holes,
·SO4-,·OH		 Catalyst = 1.5 g/L
PDS = 9 mM
AO7 = 50 mg/L		 90% degradation of AO7 in 180 min 58
Biomass Oxidant Preparation Mechanism Active sites Reactive species Reaction condition Performance ref
Pine
needle		 PMS Pyrolysis Radical Defects ·OH(main),· SO4- Catalyst = 1 g/L
PMS = 8 mM
1,4-dioxane = 20 μmol/L
Initial pH = 6.5		 84%degradation of
1,4-dioxane in 180 min		 59
Sludge
Sludge H2O2 Pyrolysis Radical sp2C, C=O,
pyridonic N and pyridinic N of PFRs		 ·OH Catalyst = 0.4 g/L
H2O2 = 1 mM
Ciprofloxacin = 10 mg/L
pH = 7		 93% degradation of
ciprofloxacin in 24 h		 60
Sludge PDS Pyrolysis Nonradical N/A Electron transfer pathway Catalyst = 0.5 g/L
PDS = 10 mM
Sulfathiazole = 20 mg/L
pH = 6		 100% removal of
sulfathiazole in 90 min		 37
Sludge PMS Pyrolysis Radical
and
Nonradical		 Fe(Ⅱ);
C=O;
defects		 ·OH, ·SO4-,1O2 Catalyst = 1 g/L
PMS = 0.8 mM
triclosan = 0.034 mM
Initial pH = 7.2		 99% degradation of
triclosan in 240 min		 61
Sludge PMS Hydrothermal coupled Pyrolysis Nonradical C=O 1O2 Catalyst = 0.4 g/L;
PMS = 0.4 g/L
sulfamethoxazole
= 0.01 g/L		 100% degradation of
sulfamethoxazole in 15 min		 22
Sludge PMS Pyrolysis Nonradical C=O 1O2 Catalyst = 0.5 g/L;
PMS = 1 mM
Bisphenol A = 1 g/L
pH = 6		 ~80% mineralization of bisphenol A in 30 min 23
Food waste
Shrimp shell PDS Pyrolysis Radical
and
Nonradical		 sp2C Electron transfer pathway
(main),
·O2-		 Catalyst = 0.2 g/L
PDS= 0.5 g/L
2,4-Dichlorophenol = 100 mg/L
Initial pH = 5.82		 76% mineralization of 2,4-dichlorophenol in 120 min 27
Swine bone PDS Pyrolysis Radical
and
Nonradical		 C=O for 1O2;
—OH for radicals		 ·OH (main),1O2, ·O2-, SO 4 · -
Electron transfer pathway		 Catalyst = 0.2 g/L
PDS= 2 g/L
2,4-Dichlorophenol = 20 mg/L		 100% degradation of 2,4-dichlorophenol in 120 min 62
Swine bone PDS Pyrolysis Radical
and
Nonradical		 —OH, —COOH for
·SO4-,·OH;
Defects, inorganic
component for 1O2, ·O2-;
C=O for ·OH, electron
transfer process		 ·SO4-,·OH,1O2, ·O2-,
Electron transfer process		 Catalyst = 0.1 g/L
PDS = 1 g/L
Acetaminophen = 20 mg/L		 100% degradation of
acetaminophen in 120 min		 62
Biomass Oxidant Preparation Mechanism Active sites Reactive species Reaction condition Performance ref
Food
waste
digestate		 PMS Pyrolysis Radical
and
Nonradical		 sp2C;
graphitic N;
pyridinium N;
C=O		 1O2, ·O2-,·OH, ·SO4- Catalyst = 0.5 g/L;
PMS= 1 mM
Reactive brilliant red X-3B = 1 g/L
Initial pH = 3.78		 >99%degradation of
X-3B in 1 min		 24
Egg shell PDS Pyrolysis Radical
and
Nonradical		 Defects and oxygen functional groups 1O2, ·O2-,·OH, ·SO4-,
Electron transfer pathway		 Catalyst = 0.167 g/L
PDS= 1 g/L
2,4-dichlorophenol= 100 mg/L		 90% removal of 2,4-Dichlorophenol in 2 h 25
Manure
Swine manure H2O2 Pyrolysis Radical PFRs ·OH(main), ·O2- Catalyst = 0.5 g/L
H2O2 = 10 mM
Sulfamethazine = 35.9 μmol/L
pH = 7.4		 > 85% degradation of
sulfamethazine in 30 min		 27
Pig manure H2O2 Pyrolysis Radical PFRs ·OH Catalyst = 0.5 g/L
H2O2 = 5 mM
Tetracycline = 67.5 μmol/L
pH = 7.4		 Nearly 100% degradation of tetracycline in 240 min 28
Alage
Enteromorpha PDS Pyrolysis Radical
and
Nonradical		 graphitic N 1O2, ·O2-, Electron transfer
pathway		 Catalyst = 0.05 g/L
PDS = 4 mM
Sulfamethoxazole = 5 mg/L		 >95% degradation of
sulfamethoxazole in 90 min		 31
Spirulina residue PDS Pyrolysis Nonradical Positively charged O near N-dopants Electron transfer pathway Catalyst = 0.5 g/L
PDS = 6 mM
Sulfamethoxazole = 20 mg/L		 100% degradation of
sulfamethoxazole in 45 min		 63
Yeast
Yeast cell (dry weight) PMS Cacination in
molten salt		 Radical
and
Nonradical		 C=O for 1O2;
sp2C, graphitic N and
pyridinic N for ·OH,
·SO4-		 1O2(main),·OH, ·SO4- Catalyst = 0.4 g/L
PMS = 0.4 g/L
Bisphenol A = 20 mg/L
pH = 7		 100% degradation of
bisphenol A in 6 min		 33
Yeast extract PMS Pyrolysis Radical
and
Nonradical		 N/A 1O2, ·O2-,·OH, ·SO4-,
Electron transfer pathway		 Catalyst = 0.05 g/L
PMS= 5.7 mM
p-Hydroxybenzoic acid = 10 ppm
pH = 4.5		 Nearly 100% degradation of p-hydroxybenzoic acid in 90 min 32
图1 生物炭活化过氧化物机理汇总
Fig. 1 The summary of the mechanism of peroxides activation by biochar
图2 PFRs的形成过程及PFRs活化过氧化物机理示意图[50,73,81]
Fig. 2 The scheme for the formation of PFRs and the mechanism of peroxides activation by PFRs[50,73,81]
图3 PFRs活化O2产生·OH机理[79]
Fig. 3 The mechanism of PFRs activating O2 to produce ·OH[79]
图4 NaCl/KCl熔融盐制备石墨化生物炭与石墨化生物炭活化PMS降解双酚A示意图(以酵母为生物质)[33]
Fig. 4 The scheme for preparation of graphitized biochar via NaCl/KCl molten salt (taking yeast as biomass) and graphitized biochar activating PMS for the degradation of Bisphenol A[33]
图5 “一锅法”制备掺氮生物炭示意图(以尿素为氮源,木屑为生物质)[72]
Fig. 5 The scheme for preparation of N-doped biochar via one-pot synthesis (taking urea as nitrogen source and wood residue as biomass)[72]
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