光催化耦合技术在废水处理中的最新进展

doi:10.1016/S1872-2067(23)64536-X

催化学报 ›› 2023, Vol. 54: 88-136.DOI: 10.1016/S1872-2067(23)64536-X

光催化耦合技术在废水处理中的最新进展

郑子叶^a, 田爽^a, 冯玉晓^a, 赵珊^a, 李鑫^b, 王曙光^a^,^c, 何作利^a^,^*()

^a山东大学环境科学与工程学院, 山东省水污染控制与资源再利用重点实验室, 山东省环境过程与健康重点实验室, 山东青岛266237
^b华南农业大学农业农村部能源植物资源与利用重点实验室, 生物质工程研究所, 广东广州510642
^c山东大学威海工业技术研究院, 山东威海264209

收稿日期:2023-07-25 接受日期:2023-09-20 出版日期:2023-11-18 发布日期:2023-11-15
通讯作者: *电子信箱: zlhe@sdu.edu.cn (何作利).
基金资助:
国家自然科学基金(22278245);山东省泰山青年学者计划(tsqn201909026);山东大学未来青年资助计划(61440089964189);山东大学青年交叉科学创新群体项目(2020QNQT014);山东省泰山特聘学者计划(tstp20230604)

Recent advances of photocatalytic coupling technologies for wastewater treatment

Ziye Zheng^a, Shuang Tian^a, Yuxiao Feng^a, Shan Zhao^a, Xin Li^b, Shuguang Wang^a^,^c, Zuoli He^a^,^*()

^aShandong Key Laboratory of Water Pollution Control and Resource Reuse, Shandong Key Laboratory of Environmental Processes and Health, School of Environmental Science and Engineering, Shandong University, Qingdao 266237, Shandong, China
^bInstitute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization, Ministry of Agriculture and Rural Affairs, South China Agricultural University, Guangzhou 510642, Guangdong, China
^cWeihai Research Institute of Industrial Technology of Shandong University, Shandong University, Weihai 264209, Shandong, China

Received:2023-07-25 Accepted:2023-09-20 Online:2023-11-18 Published:2023-11-15
Contact: *E-mail: zlhe@sdu.edu.cn (Z. He).
About author:Zuoli He (School of Environmental Science and Engineering, Shandong University) received Ph.D. in Electronic Science and Technology at Xi'an Jiaotong University in 2015. He spent one year at the University of Utah as a visiting researcher (2013-2014), two years at the Division of Environmental Science and Engineering at Pohang University of Science and Technology (POSTECH) as a postdoctoral researcher (2015-2017), and another two years at Korea Institute of Materials Science (KIMS) as a senior researcher (2017-2019). His current research interests focus on functional nanostructured composite materials for photocatalytic solar energy conversion and applications in the energy and environmental fields (including multi-technology synergistic removal of organic pollutants, pollutant sensing and monitoring technologies, photolytic hydrogen production from water, interconversion of nitrogen-containing compounds, and photothermal catalytic synthesis). He has published more than 80 peer-reviewed papers.
Supported by:
National Natural Science Foundation of China(22278245);Young Taishan Scholars Program of Shandong Province(tsqn201909026);Shandong University Future Youth Grant Program(61440089964189);Youth Interdisciplinary Science and Innovative Research Groups of Shandong University(2020QNQT014);Taishan Scholars Project of Shandong Province(tstp20230604)

摘要/Abstract

摘要：

随着工业进步和人口增长, 大量难降解的有机污染物被排放到水体中, 环境污染成为一个日益严峻的全球性问题. 大多数有机污染物具有致癌性、诱变性、细菌性和复杂多样性, 难以通过传统的化学、生物和光解等处理方法有效去除, 亟需探索环保有效的去除污染物技术. 光催化技术可以直接利用太阳光进行污染物降解, 对环境友好, 然而, 其实际应用受到太阳能利用率低、催化剂分离困难、催化剂稳定性低以及矿化率低等因素的限制. 近年来, 将光催化技术与其他技术耦合成为解决上述困难的新趋势. 对光催化耦合技术的最新进展和工作机制进行系统地梳理和总结对进一步推动去除污染物技术的发展具有重要意义.

本文系统总结了光催化耦合技术在废水处理中的最新研究进展. 首先, 简要介绍了光催化的机理和研究进展, 总结了光催化技术在废水处理过程中存在的问题. 然后, 简要介绍了光催化耦合技术在解决上述问题过程中的研究进展和发展趋势. 其后, 通过重点介绍一些典型研究, 详细地阐述了光催化技术与传统水处理技术(吸附法、膜分离法、生物降解法)、高级氧化技术(电催化法、臭氧化法、Fenton法、过硫酸盐法)和其他技术(热催化法、等离子体法、超声波法、压电催化法、磁场法)的耦合机制. 此外, 进一步探讨了光催化技术与各种技术耦合的独特优势, 概述了不同光催化耦合技术的设计原理和具体应用. 最后, 简要总结了光催化耦合技术所面临的挑战和未来的研究方向: (1) 在理论研究方面, 目前缺乏对光催化耦合技术的深入机理分析和系统的研究, 应结合光催化剂的特性并通过多种技术手段对耦合过程进行深入分析, 并深入挖掘光催化耦合机理, 以进一步指导催化剂的理性设计. (2) 目前, 光催化耦合技术研究主要集中在处理单一污染物或实验室模拟废水, 未来需要进一步开发新型稳定、高效的催化剂以满足实际生产和生活中排放的污水处理要求. (3) 应探索新型耦合技术, 可以产生更多具有强氧化能力的自由基, 以进一步提高污水处理的效率和经济可行性. (4) 传统的光催化反应器在光催化耦合体系中可能不适用, 应针对不同耦合系统探索新型反应器, 以满足大规模工业应用的需要.

综上, 本综述系统地总结了光催化耦合技术的优势、研究进展、耦合机制、设计原理、具体应用以及目前存在的挑战, 希望通过推动相关研究人员进一步思考, 并为进一步推动光催化耦合技术在废水处理领域中的实际应用, 开发高效的污染物处理技术而提供一定的参考和借鉴.

关键词: 光催化, 耦合, 技术, 协同机理, 有机污染物, 污水处理

Abstract:

As industrial advancements and population growth continue, environmental pollution has become an increasingly severe global concern. The discharge of both conventional and emergent refractory organic pollutants has led to an increasingly complex and diverse array of organic pollutants in water bodies. Photocatalysis is an environmentally friendly oxidation technology that holds significant promise for the degradation and mineralization of organic pollutants in wastewater. However, the practical application of photocatalysis is significantly limited by its low light utilization rate, challenging recovery process, and low quantum yield. To address these constraints, photocatalytic coupling technologies have emerged as a new approach. This review briefly discusses the mechanisms, research progress, and problems associated with photocatalysis for wastewater treatment. Subsequently, it provides an overview of research progress on technologies that couple photocatalysis with other water treatment technologies, and some typical research is highlighted to detail the advantages and mechanisms of various photocatalytic coupling technologies. Finally, the challenges and prospects for photocatalytic coupling technologies in wastewater treatment are presented. We hope this review will inspire more researchers to consider this important domain.

Key words: Photocatalysis, Coupling, Technology, Synergistic mechanism, Organic pollutant, Wastewater treatment

郑子叶, 田爽, 冯玉晓, 赵珊, 李鑫, 王曙光, 何作利. 光催化耦合技术在废水处理中的最新进展[J]. 催化学报, 2023, 54: 88-136.

Ziye Zheng, Shuang Tian, Yuxiao Feng, Shan Zhao, Xin Li, Shuguang Wang, Zuoli He. Recent advances of photocatalytic coupling technologies for wastewater treatment[J]. Chinese Journal of Catalysis, 2023, 54: 88-136.

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图/表 30

Fig. 1. Mechanism of photocatalysis.

Fig. 2. Photocatalyst modification strategies.

Fig. 3. Requirements for and problems with photocatalysis technologies.

Fig. 4. Photocatalytic coupling technologies.

Fig. 5. (a) Top and side views of optimized BC-MB and BC-RhB structures. (b) Photoluminescence emission spectra of prepared materials. (c) MB and RhB degradation mechanism by BC/2ZIS/WO3. Reprinted with permission from Ref. [109]. Copyright 2022, Elsevier. (d) Photocatalytic mechanism of BiOBr/Bi2MoO6@MXene under visible light irradiation. (e) Crystal structure, energy band diagrams, density, and local density of states of Bi2MoO6@MXene and BiOBr/Bi2MoO6@MXene. Reprinted with permission from Ref. [112]. Copyright 2023, Elsevier. 1,2,3-TCB degradation mechanism (f) and bacterial community composition (genus) (g) in the ICPB system. Reprinted with permission from Ref. [125]. Copyright 2022, Elsevier.

Fig. 6. (a) Degradation pathway, charge separation, and mechanism of PFOA degradation in the photoelectrocatalysis system. Reprinted with permission from Ref. [149]. Copyright 2022, Elsevier. (b) Optimal cell structures of CN, Cl-CN, and Cl/S-CN (left) and electron density diagrams of C3N4 and Cl/S-CN near the O, C, and S atoms (right). (c) Formation mechanism of ROS-rich region during the reaction and the ROS chain reaction. Reprinted with permission from Ref. [137]. Copyright 2022, Elsevier. (d) Adsorption energy and charge density of H2O2 on Bi, Bi-Fe, and Fe sites of BiOCl@Fe-BiOCl (top) and activation energy of H2O2 to ?OH transformation at various sites (bottom). Reprinted with permission from Ref. [142]. Copyright 2023, Elsevier. (e) CIP degradation mechanism by BM in concurrent photocatalysis-persulfate activation system. Reprinted with permission from Ref. [148]. Copyright 2023, Elsevier.

Fig. 7. (a) BPF degradation mechanism by CuO@NCs. (b) Optimized structure, f0, and f- (top) and three degradation pathways of BPF by CuO@NCs in the photothermal catalytic process (bottom). Reprinted with permission from Ref. [154]. Copyright 2023, Elsevier.

Fig. 8. (a) Reaction mechanism of the photocatalytic plasma reactor. (b) Mechanism of MO degradation under the combined action of O3 and photocatalysis. Reprinted with permission from Ref. [160]. Copyright 2021, Elsevier. (c) Mechanism of RhB degradation by ultrasound-assisted TiO2 photocatalysis. Reprinted with permission from Ref. [166]. Copyright 2021, Elsevier. (d) Structure and attack sites of DCF. (e) Mechanism of DCF degradation by 1T/2H MS/BWO under light, ultrasonic, and combined light/ultrasonic irradiation, and the DCF degradation pathway. Reprinted with permission from Ref. [174]. Copyright 2022, Elsevier. (f) DOS (left) and (001)-spin polarized planar 3D spatial distribution (right) of metal-deficient Ti15O32 model. (g) Degradation efficiency of different pollutants by TiO2-10 under different magnetic field intensities. Reprinted with permission from Ref. [179]. Copyright 2020, Nature Portfolio.

Fig. 9. Materials used in photocatalytic adsorption technologies.

Fig. 10. (a) SEM image of TBC-2 composite (left), ST removal capacity of TBC-2 and BC in 2 h under different conditions (middle), and schematic diagram of ST degradation by photocatalytic adsorption (right). Reprinted with permission from Ref. [183]. Copyright 2018, Wiley. (b) SEM image of BZ-25% (left), MB degradation performance of various materials during adsorption (dotted line) and coupled adsorption/photocatalysis (solid line) (middle), and mechanism of MB degradation during photocatalytic adsorption (right). Reprinted with permission from Ref. [187]. Copyright 2021, Elsevier. (c) Possible photocatalytic mechanism for multi-antibiotic removal by BC/BiOCl composite. Reprinted with permission from Ref. [189]. Copyright 2023, Elsevier. (d) Mechanism of TC degradation by g-MoS2/PGBC nanocomposite during photocatalytic adsorption. Reprinted with permission from Ref. [192]. Copyright 2022, Elsevier. (e) Removal efficiency of MB (left) and RR24 (middle) and schematic diagram of the degradation mechanism in the presence of TiO2-rGO aerogel (right). Reprinted with permission from Ref. [199]. Copyright 2023, Elsevier.

Fig. 11. (a) SEM image of ZIF-8@TiO2 composite (left), TC removal efficiency by three materials (middle), and possible photocatalytic mechanism (right). Reprinted with permission from Ref. [201]. Copyright 2020, Elsevier. (b) Preparation of 1T/2H-MoS2/ZIF-8 nanocomposites (left) and photodegradation efficiency of TC (middle) and CIP (right) by a series of 1T/2H-MoS2/ZIF-8 composites and MoS2. Reprinted with permission from Ref. [203]. Copyright 2019, Elsevier. (c) SEM images of In2S3/MIL-100(Fe) composite (left), removal rate of TC by different materials (middle), and photocatalytic mechanism (right). Reprinted with permission from Ref. [205]. Copyright 2020, Elsevier. (d) SEM (left) and TEM (middle) images of 9 wt% BiOI/MIL-125(Ti) composite and possible TC removal mechanism (right). Reprinted with permission from Ref. [210]. Copyright 2021, Elsevier.

Fig. 12. (a) Field-emission SEM images of g-C3N4/MgAl0.80Ce0.20-LDH (left), adsorption and photocatalytic capacity of various materials (middle), and reaction mechanism of g-C3N4/MgAl0.80Ce0.20-LDH in the coupling process (right). Reprinted with permission from Ref. [212]. Copyright 2022, Elsevier. (b) Reaction rate constants of RhB degradation by Zeo-ZnO and Zeo-TiO2. (c) Reaction mechanism in the coupling system. Reprinted with permission from Ref. [214]. Copyright 2020, Elsevier. (d) Mechanism of photocatalytic RhB degradation on OCN/SiNS composite. Reprinted with permission from Ref. [216]. Copyright 2022, American Chemical Society.

Fig. 13. (a) X-3B removal capacity by TiO2/Al2O3 in the coupling system (left) and cyclic performance of TiO2/Al2O3 (right). Reprinted with permission from Ref. [219]. Copyright 2019, Elsevier. (b) PFOA degradation mechanism by BN/TiO2. Reprinted with permission from Ref. [223]. Copyright 2022, Elsevier. (c) SEM images and photocatalytic degradation mechanism of MI-FC. Reprinted with permission from Ref. [225]. Copyright 2022, Elsevier.

Fig. 14. (a) Schematic diagram of PMR. Reprinted with permission from Ref. [230]. Copyright 2019, Elsevier. (b) Preparation of Ag-TiO2/PVDF-HFP membrane (left) and mechanism and stability of NOR degradation (right). Reprinted with permission from Ref. [234]. Copyright 2020, Elsevier.

Fig. 15. (a) Schematic diagram of the PMR system. Reprinted with permission from Ref. [236]. Copyright 2020, Elsevier. (b) Dead-end filtration system of the PMR. Reprinted with permission from Ref. [238]. Copyright 2019, Elsevier. (c) Cyclic E2 degradation experiments. Reprinted with permission from Ref. [239]. Copyright 2022, Elsevier. (d) Mechanism of photocatalytic activity in ZnO/multi-walled CNT mixed-matrix PES membranes. Reprinted with permission from Ref. [240]. Copyright 2017, Elsevier.

Fig. 16. (a) SM2 removal rates of BiVO4, algae, and coupled system. Asterisks represent significant differences. Reprinted with permission from Ref. [245]. Copyright 2020, Elsevier. (b) Photograph of ICPB reactor for CIP degradation. Reprinted with permission from Ref. [246]. Copyright 2023, Elsevier. (c) SMX and dissolved organic carbon removal rates of different systems. (d) Photograph of biofilm culture reactor. Reprinted with permission from Ref. [80]. Copyright 2023, Elsevier. (e) ICPB reactor and its related mechanism. Reprinted with permission from Ref. [247]. Copyright 2022, Elsevier.

Fig. 17. (a) Synergistic photocatalysis/biodegradation mechanism for PDI removal. Reprinted with permission from Ref. [248]. Copyright 2022, Elsevier. (b) Effects of photodegradation, biodegradation, and 3D semiconductor-microbial interface on p-CP and TOC removal. (c) The 3D semiconductor-microbial interface enhances the p-CP degradation mechanism. Reprinted with permission from Ref. [249]. Copyright 2022, Elsevier.

Fig. 18. (a) SEM image (left) and cross-sectional morphology (right) of Ar-Fe2O3/Ti3+-TiO2-NTs. (b) Pollutant degradation mechanism of Ar-Fe2O3/Ti3+-TiO2-NTs. (c) Removal of seven pollutants by photoelectrocatalysis using Ar-Fe2O3/Ti3+-TiO2-NTs. Reprinted with permission from Ref. [251]. Copyright 2022, Elsevier. (d) Dual photoelectrocatalysis coupling system. Reprinted with permission from Ref. [252]. Copyright 2021, Elsevier.

Fig. 19. (a) SEM images of MoS2 NTs (top) and MoS2 NT/CuInS2 QD composites (bottom). (b) TC degradation mechanism by the composite photoanode. Reprinted with permission from Ref. [254]. Copyright 2022, Elsevier. (c) Comparison of CIP degradation efficiency using different catalytic processes (left) and the photoelectrocatalytic reaction mechanism (right). Reprinted with permission from Ref. [255]. Copyright 2020, Elsevier. (d) OTC degradation mechanism of composite photoelectrode in a two-chamber photoelectrocatalysis system. Reprinted with permission from Ref. [259]. Copyright 2022, Elsevier. (e) Photographs of photoelectrocatalysis system for NOR degradation. Reprinted with permission from Ref. [258]. Copyright 2022, Elsevier.

Fig. 20. (a) ALZ and MTZ removal mechanism by photocatalytic ozonation. Reprinted with permission from Ref. [260]. Copyright 2022, Elsevier. (b) Experimental device of photocatalytic O3 system. Reprinted with permission from Ref. [261]. Copyright 2020, Elsevier. (c) Experimental setup of photocatalytic ozonation system. Reprinted with permission from Ref. [262]. Copyright 2020, Elsevier. (d) Experimental device of photocatalytic ozonation system. Reprinted with permission from Ref. [263]. Copyright 2022, Elsevier.

Fig. 21. (a) Photocatalytic ozonation coupling systems. (b) MnO2-NH2/GO/p-C3N4 design process (top), synergistic degradation mechanism (bottom left), and CLX degradation efficiency in different systems (bottom right). Reprinted with permission from Ref. [265]. Copyright 2022, Elsevier. (c) Photocatalytic ozonation coupling reactor. (d) Three-stage cyclic degradation mechanism of HSCHy-CN via photocatalytic ozonation. Reprinted with permission from Ref. [266]. Copyright 2022, Elsevier.

Fig. 22. (a) Scheme of σ-π bond formation in Fe-doped g-C3N4. (b) Phenol degradation rates of different Fenton, photocatalytic, and photo-Fenton oxidation systems. (c) Phenol removal mechanism of the photo-Fenton oxidation system. Reprinted with permission from Ref. [268]. Copyright 2019, Elsevier.

Fig. 23. (a) SEM image of Fe-BiOBr. (b) Phenol removal rate (left) and rate constant (right) in various systems. (c) Synergistic reaction mechanism of Fe-BiOBr in the photo-Fenton process. (d) Stability and Fe leaching test results. Reprinted with permission from Ref. [271]. Copyright 2023, Elsevier.

Fig. 24. (a) CIP removal rate (left) and pseudo-first-order kinetic curve (right). (b) Proposed CIP removal mechanism in the coupling process. Reprinted with permission from Ref. [278]. Copyright 2020, Elsevier. (c) LEV removal efficiency and K value of different processes. (d) Mechanism and pathway of LEV removal in the coupling process. Reprinted with permission from Ref. [279]. Copyright 2021, Elsevier.

Fig. 25. (a) TC removal efficiency of different processes. (b) Mechanism of TC removal by photocatalytic CNx/persulfate system. Reprinted with permission from Ref. [280]. Copyright 2021, Elsevier. (c) Catalytic performance of materials prepared at 400, 500, and 600 °C. (d) Fenton-like reaction mechanism by SA Fe-g-C3N4(600)/PMS. Reprinted with permission from Ref. [281]. Copyright 2022, Elsevier.

Fig. 26. (a) Schematic (left) and photograph (right) of the experimental device. (b) SEM images of 3D flower-like CuS. (c) Mechanism of MB degradation during photothermal catalysis. (d) Plots of ln(C0/Ct) vs. photocatalytic time (t). Reprinted with permission from Ref. [283]. Copyright 2018, Elsevier. (e) Synergistic photocatalytic-photothermal degradation of RhB and Ag+ by MXene membrane. (f) Kinetics of RhB removal by Ag/TCM-5 membrane under different conditions. Reprinted with permission from Ref. [284]. Copyright 2023, Elsevier.

Fig. 27. (a) Experimental device used in the photocatalytic plasma coupling system. (b) PNP removal rate in photocatalysis, plasma, and coupled photocatalysis/plasma systems within 30 min. Reprinted with permission from Ref. [288]. Copyright 2022, Elsevier. (c) Experimental device diagram. (d) Removal rate constants of photocatalysis, plasma, and coupled photocatalysis/plasma treatments. (e) CIP removal mechanism by DBD. Reprinted with permission from Ref. [289]. Copyright 2022, Elsevier. (f) Experimental setup of the coupled system. (g) Synergistic mechanism of NOR degradation by VP-Fe3O4 and UBP. Reprinted with permission from Ref. [290]. Copyright 2022, Elsevier.

Fig. 28. (a) RhB degradation by rutile TiO2 nanorods (top) and anatase TiO2 nanoflakes (bottom) under ultrasonic, visible light, and combined ultrasonic and visible light irradiation. Reprinted with permission from Ref. [292]. Copyright 2022, Royal Society of Chemistry. (b) TC removal efficiency of different systems. Reprinted with permission from Ref. [293]. Copyright 2020, Elsevier. (c) TC mineralization by C2ZO catalyst after 180 min of illumination at 20 °C and pH 8. Reprinted with permission from Ref. [294]. Copyright 2022, Elsevier. (d) Proposed mechanism of ultrasonic photocatalysis by Cu2MG composites for TC and CIP degradation. Reprinted with permission from Ref. [296]. Copyright 2021, Elsevier.

Fig. 29. (a) MO degradation ratio under different conditions. Reprinted with permission from Ref. [301]. Copyright 2020, Elsevier. (b) RhB degradation efficiency and k values under different conditions. Reprinted with permission from Ref. [303]. Copyright 2020, Elsevier. (c) Experimental device for RhB degradation via coupled piezo-photocatalysis. (d) Piezo-photocatalytic process of AO g-C3N4. Reprinted with permission from Ref. [304]. Copyright 2023, Elsevier. (e) Band scheme of equilibrium system and systems during photocatalysis, piezocatalysis, and piezo-photocatalysis. Reprinted with permission from Ref. [305]. Copyright 2022, Elsevier. (f) RhB degradation mechanism by SBTO/BOC composite in the coupled piezo-photocatalysis process and kinetic rate constants of different catalytic processes. Reprinted with permission from Ref. [306]. Copyright 2022, Elsevier. (g) RhB degradation mechanism of SBTO/Ag2O composite materials in piezo-photocatalysis process and k values of different reaction systems. Reprinted with permission from Ref. [307]. Copyright 2023, Elsevier.

Fig. 30. (a) Mechanism of coupled photocatalysis-magnetic field system. Reprinted with permission from Ref [309]. Copyright 2020, American Chemical Society. (b) Experimental device used in photocatalysis-magnetic field system. (c) Spin-dependent DOS engineering effect of Co-doped ZnO nanowire surface under an applied magnetic field. Reprinted with permission from Ref. [310]. Copyright 2021, American Chemical Society. (d) Experimental equipment of the coupling system. Reprinted with permission from Ref. [178]. Copyright 2018, American Chemical Society. (e) MO degradation efficiency by photocatalysis-magnetic field coupling system. Reprinted with permission from Ref. [311]. Copyright 2019, Wiley. (f) Device diagram of microfluidic reaction system. Reprinted with permission from Ref. [312]. Copyright 2019, Springer.

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光催化耦合技术在废水处理中的最新进展

Recent advances of photocatalytic coupling technologies for wastewater treatment

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