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

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

Chinese Journal of Catalysis ›› 2024, Vol. 61: 97-110.DOI: 10.1016/S1872-2067(24)60014-8

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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)

Abstract

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

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

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[1]	Yunhang Shao, Yaning Zhang, Chaofeng Chen, Shuai Dou, Yang Lou, Yuming Dong, Yongfa Zhu, Chengsi Pan. Enhancement of H₂O₂generation rate in porphyrin photocatalysts via crystal facets regulation to create strong internal electric field [J]. Chinese Journal of Catalysis, 2024, 61(6): 205-214.
[2]	Haoming Huang, Qingqing Lin, Qing Niu, Jiangqi Ning, Liuyi Li, Jinhong Bi, Yan Yu. Metal-free photocatalytic reduction of CO₂ on a covalent organic framework-based heterostructure [J]. Chinese Journal of Catalysis, 2024, 60(5): 201-208.
[3]	Junxian Bai, Rongchen Shen, Guijie Liang, Chaochao Qin, Difa Xu, Haobin Hu, Xin Li. Topology-induced local electric polarization in 2D thiophene-based covalent organic frameworks for boosting photocatalytic H₂ evolution [J]. Chinese Journal of Catalysis, 2024, 59(4): 225-236.
[4]	Lele Wang, Wenyao Cheng, Jiaxin Wang, Juan Yang, Qinqin Liu. Construction of intramolecular and interfacial built-in electric field in a donor-acceptor conjugated polymers-based S-scheme heterojunction for high photocatalytic H₂ generation [J]. Chinese Journal of Catalysis, 2024, 58(3): 194-205.
[5]	Yong Zhang, Junyi Qiu, Bicheng Zhu, Guotai Sun, Bei Cheng, Linxi Wang. Hollow spherical covalent organic framework supported gold nanoparticles for photocatalytic H₂O₂ production [J]. Chinese Journal of Catalysis, 2024, 57(2): 143-153.
[6]	Yucheng Jin, Xiaolin Liu, Chen Qu, Changjun Li, Hailong Wang, Xiaoning Zhan, Xinyi Cao, Xiaofeng Li, Baoqiu Yu, Qi Zhang, Dongdong Qi, Jianzhuang Jiang. Perylene diimide covalent organic frameworks super-reductant for visible light-driven reduction of aryl halides [J]. Chinese Journal of Catalysis, 2024, 57(2): 171-183.
[7]	Hao Cai, Fang Chen, Cheng Hu, Weiyi Ge, Tong Li, Xiaolei Zhang, Hongwei Huang. Oxygen vacancies mediated ultrathin Bi₄O₅Br₂ nanosheets for efficient piezocatalytic peroxide hydrogen generation in pure water [J]. Chinese Journal of Catalysis, 2024, 57(2): 123-132.
[8]	Mingjie Cai, Yanping Liu, Kexin Dong, Xiaobo Chen, Shijie Li. Floatable S-scheme Bi₂WO₆/C₃N₄/carbon fiber cloth composite photocatalyst for efficient water decontamination [J]. Chinese Journal of Catalysis, 2023, 52(9): 239-251.
[9]	Xin Liu, Maodi Wang, Yiqi Ren, Jiali Liu, Huicong Dai, Qihua Yang. Construction of modularized catalytic system for transfer hydrogenation: Promotion effect of hydrogen bonds [J]. Chinese Journal of Catalysis, 2023, 52(9): 207-216.
[10]	Qing Niu, Linhua Mi, Wei Chen, Qiujun Li, Shenghong Zhong, Yan Yu, Liuyi Li. Review of covalent organic frameworks for single-site photocatalysis and electrocatalysis [J]. Chinese Journal of Catalysis, 2023, 50(7): 45-82.
[11]	Xin Yuan, Hai-Bin Fan, Jie Liu, Long-Zhou Qin, Jian Wang, Xiu Duan, Jiang-Kai Qiu, Kai Guo. Recent advances in photoredox catalytic transformations by using continuous-flow technology [J]. Chinese Journal of Catalysis, 2023, 50(7): 175-194.
[12]	Mengistu Tulu Gonfa, Sheng Shen, Lang Chen, Biao Hu, Wei Zhou, Zhang-Jun Bai, Chak-Tong Au, Shuang-Feng Yin. Research progress on the heterogeneous photocatalytic selective oxidation of benzene to phenol [J]. Chinese Journal of Catalysis, 2023, 49(6): 16-41.
[13]	Fangpei Ma, Qingping Tang, Shibo Xi, Guoqing Li, Tao Chen, Xingchen Ling, Yinong Lyu, Yunpeng Liu, Xiaolong Zhao, Yu Zhou, Jun Wang. Benzimidazole-based covalent organic framework embedding single-atom Pt sites for visible-light-driven photocatalytic hydrogen evolution [J]. Chinese Journal of Catalysis, 2023, 48(5): 137-149.
[14]	Ning Li, Xueyun Gao, Junhui Su, Yangqin Gao, Lei Ge. Metallic WO₂-decorated g-C₃N₄ nanosheets as noble-metal-free photocatalysts for efficient photocatalysis [J]. Chinese Journal of Catalysis, 2023, 47(4): 161-170.
[15]	Zhipeng Xie, Xiubei Yang, Pei Zhang, Xiating Ke, Xin Yuan, Lipeng Zhai, Wenbin Wang, Na Qin, Cheng-Xing Cui, Lingbo Qu, Xiong Chen. Vinylene-linked covalent organic frameworks with manipulated electronic structures for efficient solar-driven photocatalytic hydrogen production [J]. Chinese Journal of Catalysis, 2023, 47(4): 171-180.