共价有机框架基光催化剂合成过氧化氢和高价值化学品的最新进展

doi:10.1016/S1872-2067(24)60014-8

催化学报 ›› 2024, Vol. 61: 97-110.DOI: 10.1016/S1872-2067(24)60014-8

共价有机框架基光催化剂合成过氧化氢和高价值化学品的最新进展

刘高雄^a, 陈润东^a, 夏兵全^a^,^*(), 吴珍^b, 刘善堂^a^,^*(), 冉景润^c^,^*()

^a武汉工程大学化学与环境工程学院, 绿色化工过程教育部重点实验室, 湖北武汉 430074, 中国
^b鄂尔多斯应用技术学院化学工程学系, 内蒙古鄂尔多斯 017000, 中国
^c阿德莱德大学化学工程学院, 阿德莱德, 澳大利亚

收稿日期:2024-01-31 接受日期:2024-03-24 出版日期:2024-06-18 发布日期:2024-06-20
通讯作者: * 电子信箱: xiab@wit.edu.cn (夏兵全), stliu@wit.edu.cn (刘善堂), jingrun.ran@adelaide.edu.au (冉景润).
基金资助:
澳大利亚研究理事会(ARC)探索项目(FT230100192);湖北省自然科学基金(2023AFB181);武汉工程大学科学基金(23QD02)

Synthesis of H₂O₂ and high-value chemicals by covalent organic framework-based photocatalysts

Gaoxiong Liu^a, Rundong Chen^a, Bingquan Xia^a^,^*(), Zhen Wu^b, Shantang Liu^a^,^*(), Amin Talebian-Kiakalaieh^c, Jingrun Ran^c^,^*()

^aKey Laboratory of Green Chemical Engineering Process of Ministry of Education, School of Chemistry and Environmental Engineering, Wuhan Institute of Technology, Wuhan 430074, Hubei, China
^bDepartment of Chemical Engineering, Ordos Institute of Technology, Ordos 017000, Inner Mongolia, China
^cSchool of Chemical Engineering, University of Adelaide, Adelaide, SA 5005, Australia

Received:2024-01-31 Accepted:2024-03-24 Online:2024-06-18 Published:2024-06-20
Contact: * E-mail: xiab@wit.edu.cn (B. Xia), stliu@wit.edu.cn (S. Liu),jingrun.ran@adelaide.edu.au (J. Ran).
About author:Bingquan Xia (School of Chemistry and Environmental Engineering, Wuhan Institute of Technology) obtained his Ph.D. degree in 2022 from the University of Adelaide in Australia. Following the completion of his doctoral studies, he joined the faculty of the School of Chemistry and Environmental Engineering at Wuhan Institute of Technology. His research is centered around the development of novel materials for photocatalysis and electrocatalysis. Specifically, he is particularly interested in the field of photocatalysis, with a focus on the conversion of solar energy into green fuels and valuable chemicals. With a strong dedication to advancing scientific knowledge, he has published 25 peer-reviewed papers.
Shantang Liu (School of Chemistry and Environmental Engineering, Wuhan Institute of Technology) Professor Shantang Liu completed his Ph.D. in the College of Chemistry and Molecular Engineering at Peking University in 2000. Following that, he pursued postdoctoral research at esteemed international institutions, including the Weizmann Institute of Science in Israel, Laval University in Canada, and Virginia Commonwealth University in the United States, from 2000 to 2007. In 2007, he joined Wuhan Institute of Technology as a full professor. Professor Liu's research interests encompass a diverse range of areas, including MEMS gas sensors, catalytic decomposition of pollutants, photothermal catalysis, energy conversion and storage. He has actively collaborated with industry partners to promote the commercialization of research outcomes and has a strong track record of publishing more than 100 peer-reviewed papers.
Supported by:
Australian Research Council (ARC) through the Discovery Project programs(FT230100192);Natural Science Foundation of Hubei Province(2023AFB181);Science Foundation of Wuhan Institute of Technology(23QD02)

摘要/Abstract

摘要：

过氧化氢(H₂O₂)广泛用于废水处理、燃料电池及漂白剂等领域. 尽管传统生产H₂O₂的蒽醌法拥有成熟的技术基础, 但存在能耗高、爆炸风险、毒气排放以及环境污染等问题. 太阳能驱动的光催化合成H₂O₂作为一种绿色、无污染、可持续的能源转换技术, 展现出替代传统的蒽醌工艺的巨大潜力. 共价有机框架(COFs)作为光催化合成H₂O₂的新兴催化剂, 以可调节的能带结构、宽光吸收范围及高光催化效率在克服传统无机光催化剂低转化效率方面显示出优势. 通过合理的结构设计调整氧还原反应(ORR)途径, COFs可提升光催化合成H₂O₂的产率, 并可同时促进高附加值化学品的合成.
本文综述了基于COFs的光催化剂在H₂O₂合成及选择性氧化高价值化学品领域的最新研究进展. 首先, 详细讨论了COFs基光催化剂在合成H₂O₂过程中的三种主要途径: (1) 单步两电子氧还原反应; (2) 两步单电子氧还原反应; (3) 双通道反应机制. 同时, 强调了牺牲剂对光催化合成H₂O₂和高附加值化学品的影响. 其次, 总结了多种新颖的COF基光催化剂合成策略, 包括静电自组装、原位合成、蒸汽辅助工艺、孔隙划分和界面聚合等, 这些策略在光催化生产H₂O₂及高价值化学品方面发挥了关键作用. 接下来, 深入探讨了提升COFs在H₂O₂和高价值化学品生成效率方面的策略, 主要包括单原子生长、异质结构建、活性位点调节和催化环境控制等四种修饰策略. 这些策略涉及材料的贵金属改性、材料相互作用促进、官能团设计以及反应界面的亲疏水性质, 旨在从整体上推动COFs在光催化的可持续性和增值化学合成方向的研究与创新. 最后, 提出了COFs基光催化剂面临的挑战与当前进展. 其中, COFs的薄膜制备和多相体系构建对于解决催化剂的分离与回收问题至关重要. 同时, 强调了机理表征在提升COF基光催化剂整体性能中的重要性.
综上, COFs基光催化剂在合成设计、反应途径的调控以及牺牲剂的引入等方面都会对合成H₂O₂和高值化学品产生重要影响. 本文旨在为构建COF基光催化剂提升整体光催化性能提供一定的参考和借鉴.

关键词: 共价有机框架, 光催化, 过氧化氢合成, 高价值化学品, 设计策略

Abstract:

Hydrogen peroxide (H₂O₂) is a versatile and environmentally friendly oxidizer widely used in diverse fields. The solar-driven photocatalytic oxygen reduction reaction generates H₂O₂ from air and water, avoiding undesirable byproducts. This green and pollution-free route is applicable to various domains. Although extensive research covers covalent organic framework (COF)-based photocatalysts for H₂O₂, little attention has been paid to systems that generate high-value chemicals in the presence of scavengers. To address this gap, we systematically discuss the simultaneous photocatalytic generation of H₂O₂ and valuable chemicals. We emphasize the pathways for H₂O₂ generation using COF-based photocatalysts and highlight the role of sacrificial agents. Novel synthetic methodologies and modification strategies for enhancing the photocatalytic yield are presented. Our work aims to strengthen the identification and discussion of the challenges faced by photocatalysts in this field. This study aims to inspire further investigations and innovations in COF-based photocatalysis for sustainable and value-added chemical synthesis by presenting a holistic view.

Key words: Covalent organic framework, Photocatalyst, H₂O₂ generation, High-value chemical, Design strategy

刘高雄, 陈润东, 夏兵全, 吴珍, 刘善堂, 冉景润. 共价有机框架基光催化剂合成过氧化氢和高价值化学品的最新进展[J]. 催化学报, 2024, 61: 97-110.

Gaoxiong Liu, Rundong Chen, Bingquan Xia, Zhen Wu, Shantang Liu, Amin Talebian-Kiakalaieh, Jingrun Ran. Synthesis of H₂O₂ and high-value chemicals by covalent organic framework-based photocatalysts[J]. Chinese Journal of Catalysis, 2024, 61: 97-110.

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图/表 13

Fig. 1. Strategies for fabricating COF-based photocatalysts toward efficient H2O2 production.

Fig. 2. Energy diagram depicting photocatalytic H2O2 production via ORR and WOR pathways.

Fig. 3. The O2 adsorption site and thickness on (a) and (b). (c) The energy required to adsorb O2 on the optimal photocatalyst locations. (d) The energetic landscape for the ORR on the surfaces of photocatalysts. (e) The photocatalytic production of H2O2 through the ORR route. Reproduced with permission from Ref. [50]. Copyright 2023, Wiley.

Fig. 4. (a,b) Photocatalyst charge differential maps. (c) The scheme of the solar-driven H2O2 generation over photocatalysts. Reproduced with permission from Ref. [30]. Copyright 2023, Science China Press.

Fig. 5. Representation of the photocatalyst structure, with yellow balls representing S atoms and blue balls representing N atoms. (a) Diagram illustrating different reaction paths for H2O2 production. (b) Charge distribution diagram of the photocatalyst, where yellow and blue regions correspond to the accumulation and depletion of thiazole charge on BT and exhaustion of S-atom charge on TTF. (c) Adsorption of *OOH and *OH on the S site of BT and S site of TTF, respectively. Reproduced with permission from Ref. [51]. Copyright 2023, Wiley.

Fig. 7. Strategies for fabricating COF-based photocatalytic materials.

Fig. 8. (a) Graphic illustrating the variation in charge density within fluorinated TAPT-TFPA@Pd ICs due to the limited availability of Pd atoms (Yellow and blue regions represent electron accumulation and depletion, respectively). (b) Illustration of the mechanism of photocatalytic H2O2 production over TAPT-TFPA@Pd ICs. Reproduced with permission from Ref. [71]. Copyright 2023, American Chemical Society.

Fig. 9. The photocatalytic process that leads to the production of H2O2 and the oxidation of FA has been examined for its underlying mechanisms. Reproduced with permission from Ref. [80]. Copyright 2023, Elsevier.

Fig. 10. (a) Schematic depiction focusing on the different active sites and their photocatalytic mechanism for generating H2O2. Reproduced with permission from Ref. [83]. Copyright 2023, Wiley. (b) Schematic representation of the photo-driven quasi-topological conversion at nitrogen cation motifs. Reproduced with permission from Ref. [35]. Copyright 2023, Wiley.

Table 1 Summary photocatalysts performance for H2O2 production.

Upgrading strategy	Photocatalysts	E_g (eV)	Light source	Reaction solution	H₂O₂production (μmol g^‒1 h^‒1)	Reaction Route	Ref.
Single-atom growth	TAPT-TFPA COFs@Pd	2.54	Xe lamp	H₂O/EtOH	2143	Ⅰ	[71]
	Mn/AB-C₃N₄	2.60	427 nm	H₂O/KOH	2230	Ⅱ	[70]
	NiSAPs-PuCN	2.51	>420 nm	H₂O	342.2	Ⅰ	[88]
	Sb-SAPC15	2.63	>420 nm	H₂O	12.4	Ⅱ	[89]
Hetero-junction construction	ZnO/TpPa-Cl	1.95	AM 1.5, 45 mW cm⁻²	H₂O/EtOH	2443	Ⅰ	[38]
	TiO₂/BTTA	2.53	350-780 nm	H₂O/FFA	740	Ⅰ	[80]
	ZnIn₂S₄/TpPa-1	2.1	400-780 nm	H₂O/EtOH	258	Ⅰ	[90]
	TpPaCl₂/BiOBr	2.09	≥420 nm	H₂O/EtOH	3749	Ⅱ	[81]
Active site regulation	TF₅₀-COF	2.54	>420 nm	H₂O/BA	1739	Ⅰ	[91]
	COF-TTA-TTTA	2.04	>420 nm	H₂O/EtOH	4347	Ⅱ & Ⅲ	[92]
	TAPB-PDA-OH	2.1	>420 nm	H₂O/EtOH	2117.6	Ⅰ	[93]
	PMCR-1	2.71	400-700 nm	H₂O/BA	5500	Ⅰ	[36]
	4PE-N-S COF	1.79	420-700 nm	H₂O/EtOH	2237	Ⅰ	[94]
	HEP-TAPT-COF	2.3	>420 nm	H₂O	1750	Ⅱ & Ⅲ	[83]
	EBA-COF	2.41	420 nm	H₂O/BA	2550	Ⅰ	[95]
	Cu₃-BT-COF	1.92	Xe lamp	H₂O/FFA	1168.75	Ⅰ	[37]
Microenvironment control	Py-Da-COF	2.53	>420 nm	H₂O/EtOH	3670	Ⅰ & Ⅲ	[47]
	TPB-DMTP-COF	2.3	>420 nm	H₂O	2882	Ⅰ	[87]
	TD-COF	2.5	400-700 nm	H₂O	4060	Ⅱ & Ⅳ	[34]
	Na-CvCN@MFGP	2.56	Xe lamp	H₂O/EtOH	375	Ⅱ	[85]

Fig. 12. Challenges and perspectives for the photocatalytic co-production of H2O2 and high-value chemicals.

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共价有机框架基光催化剂合成过氧化氢和高价值化学品的最新进展

Synthesis of H₂O₂ and high-value chemicals by covalent organic framework-based photocatalysts

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共价有机框架基光催化剂合成过氧化氢和高价值化学品的最新进展

Synthesis of H2O2 and high-value chemicals by covalent organic framework-based photocatalysts

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Synthesis of H₂O₂ and high-value chemicals by covalent organic framework-based photocatalysts