生物炭基光催化剂的制备及其降解废水中的有机污染物研究进展

doi:10.16258/j.cnki.1674-5906.2023.11.012

生态环境学报 ›› 2023, Vol. 32 ›› Issue (11): 2019-2029.DOI: 10.16258/j.cnki.1674-5906.2023.11.012

生物炭基光催化剂的制备及其降解废水中的有机污染物研究进展

赵丹丹¹^,²(), 李文健³, 江丽霞⁴, 单锐²^,^*(), 陈德珍¹, 袁浩然¹^,², 陈勇¹^,²

1.同济大学机械与能源工程学院，上海 200092
2.中国科学院广州能源研究所，广东广州 510640
3.浙江金锅锅炉有限公司，浙江金华 321042
4.中国科学院重大科技任务局，北京 100864

收稿日期:2022-09-26 出版日期:2023-11-18 发布日期:2024-01-17
通讯作者: * 单锐。E-mail: shanrui@ms.giec.ac.cn
作者简介:赵丹丹（1982年生），女，副研究员，硕士，研究方向为有机固废资源化高值化利用。E-mail: zhaodd@ms.giec.ac.cn
基金资助:
广东省科技计划项目(2021A1515012263);山东省重点研发计划项目(2022CXGC010701);广东省重点研发计划项目(2019B110209003)

Progress in the Preparation and Performance of Biochar-based Photocatalysts

ZHAO Dandan¹^,²(), LI Wenjian³, JIANG Lixia⁴, SHAN Rui²^,^*(), CHEN Dezhen¹, YUAN Haoran¹^,², CHEN Yong¹^,²

1. Tongji University, Shanghai 200092, P. R. China
2. Guangzhou Institute of Energy Conversion, Chinese Academy of Science, Guangzhou 510640, P. R. China
3. Zhejiang Jinguo Boiler Co., Ltd, Jinhua 321042, P. R. China
4. Bureau of Major R&D Programs, Chinese Academy of Sciences, Beijing, 100864, P. R. China

Received:2022-09-26 Online:2023-11-18 Published:2024-01-17

摘要/Abstract

摘要：

基于生物质热解得到生物炭材料具有发达的孔隙结构、高比表面积和电子传递效率高等性质，已经被广泛应用于化工、材料、能源、环境等研究领域。目前，由于水体中各种有机污染物的大范围增加，对人体和环境造成的安全隐患不容忽视。因此，利用绿色高效的光催化剂对有机物污染物废水进行高效处置具有重要意义。该文针对不同合成方法制备的生物炭基光催化剂对废水中各种有机污染物处置的最新研究进展进行了综述。首先对生物炭载体的不同制备方法进行了对比与分析，为后续生物炭最佳制备方式的选择提供了思路。生物炭基载体能够有效避免纳米光催化材料的团聚现象，促进光催化剂在生物炭表面的分散。因此，该文还介绍了溶胶-凝胶法、水解法、超声法和热缩聚等光催化剂的制备方法，阐述了不同制备条件对光催化降解有机污染物活性的影响机制。在此基础上，重点综述了生物炭基复合材料在去除废水中典型有机污染物（甲基橙、吉米沙星、罗丹明B、磺胺甲恶唑等）方面的应用与有效性，并且将光催化剂的反应机理总结为污染物吸附、光激发电子-空穴以及污染物催化降解3个步骤。同时，生物炭基光催化材料能够增加与污染物的接触面积与提高污染物的传质过程，从而显著提高光催化剂的催化活性。最后，从绿色、清洁、可持续的角度展望了该领域的研究重点及前景，希望该综述能为新型生物炭基催化剂的研发及其在光催化研究方面提供指导性建议。

关键词: 生物炭, 光催化, 生物质, 有机污染物, 光催化剂, 反应机理

Abstract:

Biochar derived from biomass pyrolysis have been widely used in chemical, material, energy and environmental fields due to their developed pore structure, high specific surface area and easy electron transfer properties. At present, owing to the massive increase of organic pollutants in water bodies, the potential safety hazards to the human body and environment cannot be ignored. Therefore, it is important to use green and efficient photocatalysts for the treatment of organic pollutant wastewater. This paper reviews the latest research progress on biochar-based photocatalysts prepared by different synthetic methods for the disposal of various organic pollutants in wastewater. Firstly, different preparation methods of biochar carriers were compared and analyzed, revealing the characteristics of pyrolysis, hydrothermal carbonization, and baking, and providing ideas for the selection of the best preparation method of biochar. Biochar-based composites can effectively avoid the agglomeration phenomenon of nano-photocatalytic materials and promote the dispersion of photocatalysts on the surface of biochar. Therefore, this review also introduces the methods of preparing photocatalysts such as the sol-gel method, hydrolysis method, ultrasonic method, and thermal polycondensation, and describes the influencing mechanism of different preparation conditions for the activity of photocatalytic degradation of organic pollutants. On this basis, this article focuses on the application and effectiveness of biochar carriers and biochar-based composites for the removal of typical organic pollutants (methyl orange, gemifioxacin, rhodamine B, sulfamethoxazole, etc.) from wastewater, and summarizes the reaction mechanism into three steps: pollutant adsorption, photoexcited electron-hole and pollutant catalytic degradation. Meanwhile, biochar-based photocatalytic materials can increase the contact area with pollutants and enhance the mass transfer process of pollutants, thus significantly improving the catalytic activity of photocatalysts. Finally, the research highlights and offers prospects from the perspective of being green, clean and sustainable, and it is hoped that this review will guide future development of new biochar-based catalysts and research in photocatalysis.

Key words: biochar, photocatalysis, biomass, organic pollutants, photocatalysts, reaction mechanism

中图分类号:

X705

赵丹丹, 李文健, 江丽霞, 单锐, 陈德珍, 袁浩然, 陈勇. 生物炭基光催化剂的制备及其降解废水中的有机污染物研究进展[J]. 生态环境学报, 2023, 32(11): 2019-2029.

ZHAO Dandan, LI Wenjian, JIANG Lixia, SHAN Rui, CHEN Dezhen, YUAN Haoran, CHEN Yong. Progress in the Preparation and Performance of Biochar-based Photocatalysts[J]. Ecology and Environment, 2023, 32(11): 2019-2029.

图/表 2

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催化剂	生物质	金属	应用	去除率 (Re) 和回收率 (Rc)	时间¹⁾/h	去除过程	合成过程	参考文献
TiO₂/biochar	轮胎	Ti	苯酚	Re: 99%; Rc: 99%/3次	6	吸附和NSI⁴⁾	溶胶-凝胶	Makrigianni et al., 2015
TiO₂/biochar	玉米芯	Ti	磺胺甲恶唑	Re: 91%	6	吸附和ULI⁵⁾	溶胶-凝胶	Kim et al., 2016
TiO₂/biochar	核桃壳	Ti	甲基橙	Re: 96.88%; Rc: 92.45%/5次	3.5	吸附和ULI	水解	Lu et al., 2019
TiO₂/biochar	芒草秸秆芯和软木芯	Ti	苯酚	Re: 64.1% (ULI); 33.6% (VLI) Rc: (54.1%‒64.1%)/5次 (ULI)	4	吸附和ULI, VLI	连续热解和超声	Lisowski et al., 2017
TiO₂/biochar	芦苇秸秆	Ti	磺胺甲恶唑	Re: 91.27%; Rc: (86%‒91.27%)/5次	3.5	吸附和ULI	溶胶-凝胶	Zhang et al., 2017
TiO₂/biochar	人厌槐叶萍	Ti	酸性橙7染料	Re: 90%; Rc: ~90%/6次	4	吸附和ULI	溶胶-凝胶	Silvestri et al., 2019
TiO₂/biochar	聚醚酰亚胺	Ti	酸性橙7染料	Re: 90.4%	1.5	吸附和ULI	热解	Wang et al., 2016
ZnO/ biochar	麦壳、造纸污泥	Zn	吉米沙星	Re: 96.1%; Rc: (86.1%‒96.1%)/5次	0.75	超声辐射	水热合成	Norouzi et al., 2019
TiO₂/N-biochar	鸡毛	Ti	罗丹明 B	Re: 90.91%	5	吸附和VLI	自组装交联	Li et al., 2018
N-F-TiO₂/char	轮胎	Ti	苯酚	Re: 70% (SSLI)和60% (VLI); Rc: 58%/3次 (VLI)	5 (SSLI)²⁾, 11 (VLI)³⁾	吸附和SSLI, VLI	溶胶-凝胶	Antonopoulou et al., 2017
Zn-TiO₂/ biochar	芦苇秸秆	Zn, Ti	磺胺甲恶唑	Re: 81.21%; Rc: (77.41%‒81.21%)/5次	3.5	吸附和VLI	改性溶胶- 凝胶	Xie et al., 2019
Ag-TiO₂/ biochar		Ag, Ti	甲基橙	Re: 94.9%; Rc: ~90%/5次	1	吸附和ULI	水解	Shan et al., 2020b
g-C₃N₄/ biochar	水稻秸秆	‒	罗丹明B (RhB)和甲基橙(MO)	Re: 98.2% (RhB), 92.4% (MO); Rc: ~98.2% (RhB), ~92.4% (MO)/4次	3	吸附和VLI	热缩聚法	Meng et al., 2020
g-C₃N₄/ biochar	木兰花	‒	2-巯基苯并噻唑	Re: 90.5%; Rc: (90.1%‒90.5%)/4次	1.5	吸附和VLI	超声	Zhu et al., 2018b
g-C₃N₄/ biochar	木制漂白牛皮纸浆	‒	甲醛	Re: 84.63%; Rc: ~84.63%/5次	5	VLI	一步共热法	Li et al., 2019b
g-MoS₂/ biochar	水稻秸秆	Mo	盐酸四环素	Re: 80%; Rc: (>70%)/3次	4	吸附和VLI	水解	Ye et al., 2019
Bi/Bi₂O₃/ biochar	水稻秸秆	Bi	雌激素酮	Re: 94.9%; Rc: (82.9%‒94.9%)/5次	2	吸附和ULI	超声、热解	Zhu et al., 2020
BiOCl/biochar BiOBr/biochar	‒	Bi	甲基橙	Re: 90%	2.5	VLI	一步水解	Li et al., 2016
BiOCl/biochar	竹叶	Bi	盐酸四环素	Re: 71.8%; Rc: 70%/5次	2.5	吸附和VLI	一锅法	Yan et al., 2020
Biochar@ ZnFe₂O₄/BiOBr	松花粉	Zn, Fe, Bi	环丙沙星	Re: 84%; Rc: (~84%)/4次	1.5	吸附和VLI	溶剂热合成	Chen et al., 2019
biochar@CoFe₂O₄/Ag₃PO₄	松花粉	Co, Fe, Ag	双酚A	Re: 91.12%; Rc: (73.94%‒91.12%)/4次	1.5	吸附和VLI	一锅法与原位沉淀	Zhai et al., 2020
Cu₂O-CuO@ biochar	废弃燃料和拆迁废料	Cu	活性橙29	Re: 94.12%; Rc: (~94.12%)/5次	2	吸附和ULI	水热合成	Khataee et al., 2019
CdSe/ biochar	竹子	Cd	四环素	Re: 73%; Rc: (~73%)/4次	1.83	吸附和VLI	水热和原位合成	Men et al., 2019
CuWO₄/ biochar	绿印楝叶	Cu, W	环丙沙星	Re: 97%	1.5	VLI	水热合成	Thiruppathi et al., 2020
Fe₃O₄/BiOBr/ biochar	芦苇秸秆	Fe, Bi	卡马西平	Re: 95.51%; Rc: (90.15%‒95.51%)/5次	4	吸附和VLI	一步水解法和超声	Li et al., 2019a
Fe₃O₄/BiVO₄/ biochar	喜马拉雅长叶松	Fe, Bi, V	对羟基安息香酸甲酯	Re: 97.4%; Rc: (68.24%‒92.11%)/6次	3	吸附和NSI	共沉淀和原位合成	Kumar et al., 2017

催化剂	生物质	金属	应用	去除率 (Re) 和回收率 (Rc)	时间¹⁾/h	去除过程	合成过程	参考文献
TiO₂/biochar	轮胎	Ti	苯酚	Re: 99%; Rc: 99%/3次	6	吸附和NSI⁴⁾	溶胶-凝胶	Makrigianni et al., 2015
TiO₂/biochar	玉米芯	Ti	磺胺甲恶唑	Re: 91%	6	吸附和ULI⁵⁾	溶胶-凝胶	Kim et al., 2016
TiO₂/biochar	核桃壳	Ti	甲基橙	Re: 96.88%; Rc: 92.45%/5次	3.5	吸附和ULI	水解	Lu et al., 2019
TiO₂/biochar	芒草秸秆芯和软木芯	Ti	苯酚	Re: 64.1% (ULI); 33.6% (VLI) Rc: (54.1%‒64.1%)/5次 (ULI)	4	吸附和ULI, VLI	连续热解和超声	Lisowski et al., 2017
TiO₂/biochar	芦苇秸秆	Ti	磺胺甲恶唑	Re: 91.27%; Rc: (86%‒91.27%)/5次	3.5	吸附和ULI	溶胶-凝胶	Zhang et al., 2017
TiO₂/biochar	人厌槐叶萍	Ti	酸性橙7染料	Re: 90%; Rc: ~90%/6次	4	吸附和ULI	溶胶-凝胶	Silvestri et al., 2019
TiO₂/biochar	聚醚酰亚胺	Ti	酸性橙7染料	Re: 90.4%	1.5	吸附和ULI	热解	Wang et al., 2016
ZnO/ biochar	麦壳、造纸污泥	Zn	吉米沙星	Re: 96.1%; Rc: (86.1%‒96.1%)/5次	0.75	超声辐射	水热合成	Norouzi et al., 2019
TiO₂/N-biochar	鸡毛	Ti	罗丹明 B	Re: 90.91%	5	吸附和VLI	自组装交联	Li et al., 2018
N-F-TiO₂/char	轮胎	Ti	苯酚	Re: 70% (SSLI)和60% (VLI); Rc: 58%/3次 (VLI)	5 (SSLI)²⁾, 11 (VLI)³⁾	吸附和SSLI, VLI	溶胶-凝胶	Antonopoulou et al., 2017
Zn-TiO₂/ biochar	芦苇秸秆	Zn, Ti	磺胺甲恶唑	Re: 81.21%; Rc: (77.41%‒81.21%)/5次	3.5	吸附和VLI	改性溶胶- 凝胶	Xie et al., 2019
Ag-TiO₂/ biochar		Ag, Ti	甲基橙	Re: 94.9%; Rc: ~90%/5次	1	吸附和ULI	水解	Shan et al., 2020b
g-C₃N₄/ biochar	水稻秸秆	‒	罗丹明B (RhB)和甲基橙(MO)	Re: 98.2% (RhB), 92.4% (MO); Rc: ~98.2% (RhB), ~92.4% (MO)/4次	3	吸附和VLI	热缩聚法	Meng et al., 2020
g-C₃N₄/ biochar	木兰花	‒	2-巯基苯并噻唑	Re: 90.5%; Rc: (90.1%‒90.5%)/4次	1.5	吸附和VLI	超声	Zhu et al., 2018b
g-C₃N₄/ biochar	木制漂白牛皮纸浆	‒	甲醛	Re: 84.63%; Rc: ~84.63%/5次	5	VLI	一步共热法	Li et al., 2019b
g-MoS₂/ biochar	水稻秸秆	Mo	盐酸四环素	Re: 80%; Rc: (>70%)/3次	4	吸附和VLI	水解	Ye et al., 2019
Bi/Bi₂O₃/ biochar	水稻秸秆	Bi	雌激素酮	Re: 94.9%; Rc: (82.9%‒94.9%)/5次	2	吸附和ULI	超声、热解	Zhu et al., 2020
BiOCl/biochar BiOBr/biochar	‒	Bi	甲基橙	Re: 90%	2.5	VLI	一步水解	Li et al., 2016
BiOCl/biochar	竹叶	Bi	盐酸四环素	Re: 71.8%; Rc: 70%/5次	2.5	吸附和VLI	一锅法	Yan et al., 2020
Biochar@ ZnFe₂O₄/BiOBr	松花粉	Zn, Fe, Bi	环丙沙星	Re: 84%; Rc: (~84%)/4次	1.5	吸附和VLI	溶剂热合成	Chen et al., 2019
biochar@CoFe₂O₄/Ag₃PO₄	松花粉	Co, Fe, Ag	双酚A	Re: 91.12%; Rc: (73.94%‒91.12%)/4次	1.5	吸附和VLI	一锅法与原位沉淀	Zhai et al., 2020
Cu₂O-CuO@ biochar	废弃燃料和拆迁废料	Cu	活性橙29	Re: 94.12%; Rc: (~94.12%)/5次	2	吸附和ULI	水热合成	Khataee et al., 2019
CdSe/ biochar	竹子	Cd	四环素	Re: 73%; Rc: (~73%)/4次	1.83	吸附和VLI	水热和原位合成	Men et al., 2019
CuWO₄/ biochar	绿印楝叶	Cu, W	环丙沙星	Re: 97%	1.5	VLI	水热合成	Thiruppathi et al., 2020
Fe₃O₄/BiOBr/ biochar	芦苇秸秆	Fe, Bi	卡马西平	Re: 95.51%; Rc: (90.15%‒95.51%)/5次	4	吸附和VLI	一步水解法和超声	Li et al., 2019a
Fe₃O₄/BiVO₄/ biochar	喜马拉雅长叶松	Fe, Bi, V	对羟基安息香酸甲酯	Re: 97.4%; Rc: (68.24%‒92.11%)/6次	3	吸附和NSI	共沉淀和原位合成	Kumar et al., 2017

生物炭基光催化剂的制备及其降解废水中的有机污染物研究进展

Progress in the Preparation and Performance of Biochar-based Photocatalysts

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