基于共价有机框架的光催化剂的研究进展: 原理、设计和应用

doi:10.1016/S1872-2067(24)60184-1

催化学报 ›› 2025, Vol. 70: 142-206.DOI: 10.1016/S1872-2067(24)60184-1

基于共价有机框架的光催化剂的研究进展: 原理、设计和应用

董红军^a, 屈春宏^a, 李春梅^a, 胡博^b^,^*(), 李鑫^c^,^*(), 梁桂杰^e, 江吉周^d^,^*()

^a江苏大学化学化工学院, 绿色化学与化工技术研究院, 江苏省绿色新材料与新能源化学工程实验室, 江苏镇江 212013
^b白城师范学院, 吉林白城 137000
^c生物质工程研究院, 农业农村部能源植物资源与利用重点实验室, 生物基材料与能源教育部重点实验室, 华南农业大学材料与能源学院，广东广州 510642
^d武汉工程大学环境生态与生物工程学院, 绿色化工过程教育部重点实验室,磷资源开发利用教育部工程研究中心, 湖北武汉 430205
^e湖北文理学院, 低维光电材料与器件湖北省重点实验室, 湖北襄阳 441053

收稿日期:2024-09-19 接受日期:2024-11-05 出版日期:2025-03-18 发布日期:2025-03-20
通讯作者: * 电子信箱: hubo93@bcnu.edu.cn (胡博),xinli@scau.edu.cn (李鑫),027wit@163.com (江吉周).
基金资助:
国家自然科学基金(52072153);国家自然科学基金(52202238);国家自然科学基金(62004143);湖北省重点研发计划(2022BAA084);中国博士后科学基金(2021M690023);镇江重点研发计划(SH2021021)

Recent advances of covalent organic frameworks-based photocatalysts: Principles, designs, and applications

Hongjun Dong^a, Chunhong Qu^a, Chunmei Li^a, Bo Hu^b^,^*(), Xin Li^c^,^*(), Guijie Liang^e, Jizhou Jiang^d^,^*()

^aAdvanced Chemical Engineering Laboratory of Green Materials and Energy of Jiangsu Province, Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^bBaicheng Normal University, Baicheng 137000, Jilin, China
^cInstitute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization of Ministry of Agriculture and Rural Affairs, Key Laboratory for Biobased Materials and Energy of Ministry of Education, College of Materials and Energy, South China Agricultural University, Guangzhou 510642, Guangdong, China
^dSchool of Environmental Ecology and Biological Engineering, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Wuhan Institute of Technology, Wuhan 430205, Hubei, China
^eHubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang 441053, Hubei, China

Received:2024-09-19 Accepted:2024-11-05 Online:2025-03-18 Published:2025-03-20
Contact: * E-mail: hubo93@bcnu.edu.cn (B. Hu),xinli@scau.edu.cn (X. Li),027wit@163.com (J. Jiang).
About author:Bo Hu received his Ph.D. degree from Jiangsu University in 2024. Since July 2024, he has been working at the School of Chemistry, Baicheng Normal University. His research interest mainly focuses on the photo/electrocatalytic application of nanomaterials, particularly the photo/electrocatalytic conversion for hydrogen evolution and CO₂ reduction. He has published more than 20 peer-reviewed papers.
Xin Li (South China Agricultural University) received his B.S. and Ph.D. degrees in chemical engineering from Zhengzhou University in 2002 and the South China University of Technology in 2007, respectively. Then, he joined the South China Agricultural University as a faculty staff member, and became a professor in 2017. During 2012 and 2019, he worked as a visiting scholar at the Electrochemistry Center, the University of Texas at Austin, and the Department of Chemistry, the University of Utah, respectively. His research interests include photocatalysis, photoelectrochemistry, adsorption, biomass engineering and related materials, and device development.
Jizhou Jiang is currently a full Professor in School of Environmental Ecology and Biological Engineering, Wuhan Institute of Technology (WIT). He completed his PhD in the Huazhong University of Science & Technology (HUST) in 2015. This was followed by a period of postdoctoral research at National University of Singapore under the supervision of Prof. Andrew T. S. Wee from 2015 to 2017. His current research focuses on the fabrication of novel 2D carbon-based materials and their applications of photo/electro‐catalysis.
Supported by:
National Natural Science Foundation of China(52072153);National Natural Science Foundation of China(52202238);National Natural Science Foundation of China(62004143);Key R&D Program of Hubei Province(2022BAA084);Postdoctoral Science Foundation of China(2021M690023);Zhenjiang Key R&D Programmes(SH2021021)

摘要/Abstract

摘要：

随着人类社会的不断发展, 化石能源消耗日益加剧, 这不仅导致了能源短缺, 还加剧了环境问题. 为了应对这些挑战, 亟需探索清洁、绿色的新型能源转换技术. 在此背景下,光催化技术因其能将丰富的太阳能转化为化学能而广受关注. 在光催化技术中, 光催化剂的性能至关重要. 因此, 开发新型、高效的光催化剂成为提高光催化效率的关键. 然而, 传统的无机半导体材料往往存在光响应范围窄、太阳能利用率低以及光生载流子复合快等问题. 相比之下, 共价有机框架(COFs)作为一种新型的多孔聚合物材料, 其结构具有可调谐性、预设计性、丰富的孔结构、高结晶度以及快速的电荷载流子转移等特性. 这些特性使COFs材料在光催化过程中能够高效捕获和利用光能, 促进光生载流子的分离和迁移, 进而提高光催化效率. 因此, 本文对当前COF基光催化剂的研究现状进行了系统的梳理和总结, 以期推进COFs材料在光催化领域的发展和应用.

本文系统地总结了COF基催化剂在光催化领域的研究进展. 首先, 概述了COF材料在光催化领域的应用背景及其研究发展历程. 随后, 从COF基光催化剂的基本原理和特性出发, 阐述了光催化的基本机制. 接着, 总结了COF基光催化剂的主要合成方法, 包括原位生长法、自组装法和原位聚合法, 并指出了这些方法的优势, 同时梳理了COF材料的设计思路. 在光催化反应中, 激子解离是光催化反应的关键步骤. 因此, 在上述基础上, 深入探讨了增强COF基光催化剂激子的解离策略, 这些策略涵盖调节构筑单元、设计内部电子给体-受体(D-A)结构、引入表面官能团、改善π电子相互作用以及电子结构调控等. 此外, 详细讨论了针对COF基光催化剂的工程改性策略, 旨在进一步提升其光催化活性, 并对内部激发动力学以及光催化反应路径的探索进行了详细的总结和分析. 同时, 还总结了COF基光催化剂在多个光催化领域的应用, 包括分解水制氢、二氧化碳还原、过氧化氢生产、固氮、有机物转化和污染物降解等. 最后, 针对目前的研究现状, 对COF基光催化剂未来发展面临的挑战进行了简要总结: (1)电荷传输速率限制问题依然存在; (2)难以同时确保结晶度与稳定性的双重优势; (3)具有新型空间维度和结构的COF材料仍有待开发; (4)对于具体光催化机制的深入探究仍需加强.

综上所述, 本文全面总结了近年来COF材料在光催化领域的研究进展, 涵盖了COF材料在光催化领域的研究发展历程、基本原理及构建思路、合成及改性策略、在光催化各领域的实际应用, 以及面临的挑战、应用前景与未来发展方向, 以期为COF基光催化剂的未来进一步发展提供参考和借鉴.

关键词: 共价有机框架, 光催化, 结构特征, 能量转化, 环境净化

Abstract:

Covalent organic frameworks (COFs) semiconductor materials have garnered significant attention in solar to chemical energy conversion owing to their unique properties, including structural tunability, pre-design capability, large surface area, abundant pore structures, high crystallinity, excellent chemical stability, suitable energy-band structure, fast charge carrier transfer and so on. These intrinsic features endow COFs with the remarkable candidates for various photocatalytic applications including photocatalytic H₂ generation from water reduction, CO₂ reduction, degradation of organic pollutants, N₂ fixation, H₂O₂ evolution, and even organic synthesis. Here, this review comprehensively summarizes the recent advancements in COF-based materials for the above photocatalytic reactions, including the historic overview of the COF in the photocatalysis field, the fundamentals and design philosophy of COF-based photocatalysts, the advances of synthesis strategies, the structural characteristics and diversities, the practical applications in various photocatalytic fields as well as the challenges and future development direction in terms of COFs material and application perspectives. We sincerely hope this review can offer symbolic guidelines for future development COF semiconductor materials in this promising field.

Key words: Covalent organic framework, Photocatalysis, Structural feature, Energy conversion, Environmental purification

董红军, 屈春宏, 李春梅, 胡博, 李鑫, 梁桂杰, 江吉周. 基于共价有机框架的光催化剂的研究进展: 原理、设计和应用[J]. 催化学报, 2025, 70: 142-206.

Hongjun Dong, Chunhong Qu, Chunmei Li, Bo Hu, Xin Li, Guijie Liang, Jizhou Jiang. Recent advances of covalent organic frameworks-based photocatalysts: Principles, designs, and applications[J]. Chinese Journal of Catalysis, 2025, 70: 142-206.

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图/表 37

Fig. 1. (a) Statistics on the number of publications on COFs photocatalysis since 2014 (Source: Web of Science, CNKI). (b) Periods of COFs photocatalysis development and their characteristics.

Fig. 2. Development timeline of COFs. Reprinted with permission from Ref. [106]. Copyright 2005, American Association for the Advancement of Science. Reprinted with permission from Ref. [113]. Copyright 2014, Royal Society of Chemistry. Reprinted with permission from Ref. [114]. Copyright 2018, Nature Publishing Group. Reprinted with permission from Ref. [118]. Copyright 2019, Nature Publishing Group. Reprinted with permission from Ref. [120]. Copyright 2020, American Chemical Society. Reprinted with permission from Ref. [116]. Copyright 2021, Nature Publishing Group. Reprinted with permission from Ref. [117]. Copyright 2022, American Chemical Society. Reprinted with permission from Ref. [121]. Copyright 2023, Elsevier. Reprinted with permission from Ref. [119]. Copyright 2024, Wiley.

Fig. 3. Fundamentals of COF-based photocatalysts.

Fig. 4. Schematic photocatalytic reaction mechanism over COFs materials.

Fig. 5. (a) The synthesis illustration of Ni12P5/TpPa-1-COF composite. Reprinted with permission from Ref. [177]. Copyright 2022, Wiley. (b) The synthesis illustration of SDD-COFs. Reprinted with permission from Ref. [178]. Copyright 2024, Wiley. (c) The synthesis illustration of CF/TSx samples. Reprinted with permission from Ref. [179]. Copyright 2023, Wiley. (d) The synthesis illustration of CNF@COF nanopaper samples. Reprinted with permission from Ref. [180]. Copyright 2023, American Chemical Society.

Fig. 6. Design strategies and considerations of COF-based photocatalysts.

Fig. 7. Versatile properties of COF-based photocatalysts. The inserted figures are reprinted with permission from Ref. [188]. Copyright 2024, American Association for the Advancement of Science. Ref. [189]. Copyright 2023, American Chemical Society. Reprinted with permission from Ref. [190]. Copyright 2024, Nature Publishing Group. Reprinted with permission from Ref. [191]. Copyright 2024, American Chemical Society. Reprinted with permission from Ref. [192]. Copyright 2023, Wiley. Reprinted with permission from Ref. [116]. Copyright 2021, Nature Publishing Group.

Fig. 8. Strategy for strengthening exciton dissociation of COF-based photocatalysts.

Fig. 9. (a) Schematic preparation of three different imine-linked COFs. Reprinted with permission from Ref. [231]. Copyright 2018, Elsevier. (b) Schematic representation of the conversion of BT-COFs-x to TP-COFs-y via enol-ketones. Reprinted with permission from Ref. [232]. Copyright 2023, Wiley.

Fig. 10. (a) Schematics of hexavalent electron donor-acceptor COFs. Reprinted with permission from Ref. [237]. Copyright 2024, Nature Publishing Group. (b) Building blocks and synthesis flowchart of Co-Por-COFs. Reprinted with permission from Ref. [238]. Copyright 2023, Wiley. (c) Schematic diagram of the preparation of PyPz-COF. (d) Rhombic macrocyclic reconstruction structure. (e) Schematic of layer spacing, and (f) Geometry and energy-minimized cell of PyPz-COF (light blue-C; dark blue-N; white-H). Reprinted with permission from Ref. [239]. Copyright 2023, Wiley.

Fig. 11. (a) Schematic synthesis of FOO(X)-COFs. (b-d) Crystal structures of FOOBr-COF, FOOMe-COF and FOOPh-COF. Reprinted with permission from Ref. [244]. Copyright 2024, Wiley. (e) Schematic representation of carrier transport in polar functional group-functionalized COFs. Reprinted with permission from Ref. [245]. Copyright 2024, Wiley. (f) Schematic synthesis of the COF-366(Ni)-R (?R = ?CN, ?CF3 ?COOMe, ?H, and ?OMe). Reprinted with permission from Ref. [246]. Copyright 2024, Wiley.

Fig. 12. (a) The Synthesis and structural schematics. (b) UV-vis DRS. (c) Transient current responses. (d) EIS Nyquist plots. (e) The corresponding time-resolved photoluminescence spectra of Ph-COF-AO, Th-COF-AO and TTh-COF-AO samples. Reprinted with permission from Ref. [250]. Copyright 2023, Wiley. (f) The scheme for the synthesis of H-COF and ODA-COF. (g) Top and side views for AA stacking model of ODA-COF. (h) UV/Vis DRS. (i) Steady-state PL spectra. (j) EPR spectra in the dark and light condition and (k) Transient current responses of H-COF and ODA-COF. Reprinted with permission from Ref. [251]. Copyright 2022, Wiley.

Fig. 13. (a) Schematic diagram of the reverse ESIPT process from ketone to enol, photoisomerization of (b) BT-COF-2 and (c) BT-COF-3. (d) Possible ESIPT mechanism for BT-COF-2. Reprinted with permission from Ref. [255]. Copyright 2023, Wiley. The ESP of (e) SQ-COF-1, (f) SQ-COF-2, and (g) PDA-COF in the ground state. The ESP distribution maps of (h) SQ-COF-1, (i) SQ-COF-2, and (j) PDA-COF in the ground state. Reprinted with permission from Ref. [256]. Copyright 2021, Wiley. (k) Synthesized schematic and partially enlarged structures of 1D PyTTA-COF and 2D PyTTA-COF. Reprinted with permission from Ref. [257]. Copyright 2023, Wiley.

Fig. 14. Design strategies of COF-based photocatalysts.

Fig. 15. (a) Schematic design of 2D NL COFs for photocatalytic overall water splitting. Optimized structures of I-TST (b), Ai-TST (c), and Ao-TST COFs (d). (e) The calculated energy band positions of 2D COFs. Reprinted with permission from Ref. [120]. Copyright 2020, American Chemical Society. (f) Schematic of preparation and charge transfer of AuSP/COFs and AuCP/COFs. (g) UV-vis absorption curves and (h) their corresponding Tauc plots of TAPB-DMTA-COFs and Au/COFs composites. Reprinted with permission from Ref. [261]. Copyright 2020, Elsevier.

Fig. 16. (a) Structure of CotPP-CoBpy3 COF. (b) AFM image and the height profile along the marked white line. (c) Cryo-TEM pattern (insert: selected-area electron diffraction pattern). (d) High-resolution cryo-TEM images of CotPP-CoBpy3. Reprinted with permission from Ref. [264]. Copyright 2024, American Association for the Advancement of Science. (e) Schematic synthesis of UCOF-SCAU-2. Reprinted with permission from Ref. [265]. Copyright 2023, Wiley. (f) Chemical structures of COT-X-Y (X = N, O, or S; Y = C or N). (g) Schematic structures of the cyclooctatetrathiophene (COTh, COT-S-C) molecule. (h) HOMO and first orbital below the HOMO (HOMO-1) of COTh. (i) Schematic representation of the construction of a 3D FC-COF from a COT molecule (Node). Reprinted with permission from Ref. [266]. Copyright 2023, American Chemical Society.

Fig. 17. (a) Schematic representation of the topology of the (3,6)-connected eea and spn and their corresponding chemical equivalents. Reprinted with permission from Ref. [267]. Copyright 2022, Elsevier. (b) Synthesis schematic of NKCOF-25-X. Reprinted with permission from Ref. [268]. Copyright 2022, Elsevier. (c) Synthetic design routes of TBD-COF and TBC-COF. Reprinted with permission from Ref. [206]. Copyright 2024, Wiley.

Fig. 18. (a) Schematic representation of COF-topological quantum material nano-heterostructure and application. (b) Representation of the AA stacking model for COF along crystallographic c-direction and a-direction. (c) N2 adsorption and desorption isotherm profiles. (d) Calculated pore size distribution profile by NLDFT method of COF and COF-TI. Reprinted with permission from Ref. [269]. Copyright 2024, Wiley. (e) Molecular Structures of HFPTP as a six-connected 3D-D3h central building block. (f) TAPP-M as a co-quadruplex four-connected 2D-D4h monomer. (g) Structures of 3D COFs, JUC-640-M (M = H, Co, or Ni). Expanded Framework for JUC-640-M (h) and stp Net (i). N2 adsorption-desorption isotherms of JUC-640-H (j), JUC-640-Co (k), and JUC-640-Ni (l) (inset: pore-size distribution profiles). Reprinted with permission from Ref. [270]. Copyright 2023, American Chemical Society. (m) Synthesis of PEBP-COF and PETZ-COF. (n) Nitrogen adsorption isotherm of PETZ-COF (inset: pore size distribution). (o) SEM image of PETZ-COF. (p,q) HRTEM images of PETZ-COF. Reprinted with permission from Ref. [271]. Copyright 2022, Royal Society of Chemistry.

Fig. 19. (a) Schematic synthesis diagram of TBC hybrid material. Reprinted with permission from Ref. [272]. Copyright 2019, Elsevier. (b) Schematic synthesis diagram of Pd doped TiATA@LZU1 core-shell structure. Reprinted with permission from Ref. [273]. Copyright 2018, Wiley. (c) Schematic synthesis diagram of PCN-222-Cu@TpPa-1 hybrid material. Reprinted with permission from Ref. [274]. Copyright 2023, Elsevier.

Fig. 20. (a) Schematic diagram of APTES-TiO2@TMP and APTES-TiO2@TM synthesis. (b) Direct Z-scheme system photocatalysis mechanism. Reprinted with permission from Ref. [278]. Copyright 2023, Elsevier. (c) Schematic diagram of NCTS synthesis. (d) Schematic representation of the relative energy band positions and charge transfer of D-TiO2 and NH2-T-COF. Reprinted with permission from Ref. [279]. Copyright 2023, Elsevier. (e) Schematic diagram of the formation of ZT heterojunction. (f) The S-scheme photocatalytic mechanism of ZT heterojunction. Reprinted with permission from Ref. [280]. Copyright 2022, Elsevier. (g) Schematic diagram of the synthesis of Rh-COFBpy@HCOF. (h) S-scheme transfer mechanism between HCOF and Rh-COFBpy. Reprinted with permission from Ref. [281]. Copyright 2023, American Chemical Society.

Fig. 21. (a) Schematic diagram of the preparation of TAA/TAB-CTP-COF. (b) Steady-state PL measurements. (c) Transient photocurrent response. (d) Band-structure diagram. Reprinted with permission from Ref. [296]. Copyright 2024, American Chemical Society. (e) Schematic diagram of redox molecular junction COFs coupled to H2O2 photosynthesis and FFA photooxidation. (f) Steady-state PL measurements. (g) Transient photocurrent response. (h) Band structure diagram. Reprinted with permission from Ref. [297]. Copyright 2023, Wiley. (i) Schematic diagram of the preparation of 2D PTCOF. (j) Post-modification pathway of PTCOF. PL spectra (k), transient photocurrent response (l), and schematic energy band structures (m) of PTCOF, PTCOF-OID, and PTCOF-FO. Reprinted with permission from Ref. [298]. Copyright 2023, Wiley.

Fig. 22. (a) Schematic synthesis of Fe SAS/Tr-COFs. Reprinted with permission from Ref. [299]. Copyright 2022, American Chemical Society. (b) Schematic of the self-assembly synthesis process of LaNi-Phen/COF-5. (c) Schematic representation of the CO2 photoreduction over LaNi-Phen/COF-5. Reprinted with permission from Ref. [300]. Copyright 2023, Nature Publishing Group. (d) Schematic diagram of TAPT-PBA COFs@Pd IC and TAPT-TFPA COFs@Pd IC. Reprinted with permission from Ref. [301]. Copyright 2023, American Chemical Society.

Fig. 23. (a) Schematic of the synthesis of molecular analog and Py-Bde-COF and the rhombic structure of Py-Bde-COF. Reprinted with permission from Ref. [117]. Copyright 2022, American Chemical Society. (b) Schematic of the synthesis of COF-JLU35 and COF-JLU36. Reprinted with permission from Ref. [304]. Copyright 2023, American Chemical Society. (c) Schematic of the synthesis of PMCR-1. Reprinted with permission from Ref. [305]. Copyright 2023, Wiley.

Fig. 24. (a) Schematic synthesis. (b) N2 sorption isotherms (inset: pore size distribution). (c) The sorption isotherms of CO2 and N2 at 298 K. (d) Isosteric heat of CO2 of TD-COF and Ni-PCD@TD-COF. (e) In situ FTIR spectra of CO2, Ni-PCD@TD-COF in the CO2 atmosphere and after the release of CO2. (f) The steady-state PL spectra of the reaction system. (g) Time-resolved PL decay spectra of the reaction system without and with the addition of Ni-PCD@TD-COF. (h) UV-vis DRS spectrum of TD-COF and Ni-PCD@TD-COF. (i) Schematic energy-level diagram of the electron transfer between [Ru(bpy)3]Cl2 and Ni-PCD@TD-COF. Reprinted with permission from Ref. [306]. Copyright 2020, Wiley. (j) Schematic synthesis of GQDs/TpPa-1-COF. N2 sorption isotherms (k), pore size distribution (l), steady-state PL spectra (m), transient photocurrent responses (n), EIS Nyquist plots (o), and LSV curves (p) of TpPa-1 and GQDs/TpPa-1-COFs. (q) Schematic representation of the energy band positions and Fermi energy levels of TpPa-1-COF before and after contact with GQDs. Reprinted with permission from Ref. [307]. Copyright 2023, Elsevier.

Fig. 25. (a) Time slices of the TAS for COF 4P (at λex = 450 nm). (b) TAS and fitting curves of COF 4P (at λex = 450 nm). Reprinted with permission from Ref. [309]. Copyright 2023, Wiley. (c) Pseudocolor plots and (d) fs-TA spectra of 20COFIS. Reprinted with permission from Ref. [310]. Copyright 2024, Wiley. TAS (at λex = 339 nm) of FS-OH-COF (e), FS-OHOMe-COF (f), and FS-OMe-COF (g). Reprinted with permission from Ref. [59]. Copyright 2024, Wiley.

Fig. 26. (a,b) In‐situ DRIFT spectra of AT-1 under mixed atmosphere. Reprinted with permission from Ref. [311]. Copyright 2024, Elsevier. (c) In situ DRIFTS spectra of the photoenzymatic process for FDH@COF-V2-Rh. Reprinted with permission from Ref. [312]. Copyright 2024, American Chemical Society. (d) In situ FT-IR spectra of CoPc-BTM-COF. (e) Free energy schemas for 2e- (orange line) and 4e- (cyan line) ORR processes on CoPc. Reprinted with permission from Ref. [313]. Copyright 2022, American Chemical Society. (f) Free-energy schemas for H2 halogen substituted carbon of Py-XTP-BT-COFs. Reprinted with permission from Ref. [314]. Copyright 2020, Wiley. (g) Free energy diagrams for the TPCBP X-COFs. Reprinted with permission from Ref. [315]. Copyright 2023, American Chemical Society. (h) DFT-calculated relative energy profile for the reaction path. Reprinted with permission from Ref. [316]. Copyright 2024, Elsevier.

Fig. 27. Application of COF materials in photocatalysis field.

Table 1 COF-based photocatalysts applied in photocatalytic water splitting.

Photocatalyst	Light source	Sacrificial agent	Co-photocatalyst	Pro- duct	Yield (μmol g^‒1 h^‒1)	AQE (or AQY)	Stability	Characteristic	Ref.
En_TAPT-TDOEB	300W Xe lamp (λ ≥ 420 nm)	ascorbic acid	Pt (3 wt%)	H₂	~2396	None	48 h	highly stable enaminone-linked	[211]
NH₂-UiO-66@TFPT-DETH	300W Xe lamp (λ > 420 nm)	none	Pt (7.5 wt%)	H₂	7.178 × 10³	1.11% λ = 420 nm	12 h	synergistic effect within hetero-framework	[335]
Py-ClTP- BT-COF	300W Xe lamp (λ > 420 nm)	ascorbic acid	Pt (5 wt%)	H₂	8875	8.45% λ = 420 nm	48 h	Halogen modulation at the photoactive benzothiadiazole moiety	[314]
USTB-10	300W Xe lamp (λ ≥ 420 nm)	Aa	Pt (3 wt%)	H₂	21.8 × 10³	0.68% λ = 420 nm	20 h	bigger pore size	[208]
DCNA-1_AC	300W Xe lamp (λ > 420 nm)	AC	Pt (8 wt%)	H₂	27.9 × 10³	1.49% λ = 420 nm	none	linkage isomerism	[336]
TpPa(Δ)- Cu(II)-COF	300W Xe lamp (λ > 420 nm)	L-cysteine	none	H₂	14.72 × 10³	0.78% λ = 600 nm	24 h	the enantioselective binding of the chiral COF-Cu(II) backbone to L-/D-cysteine sacrificial donors	[337]
g-C₄₀N₃-COF	300W Xe lamp (λ > 420 nm)	TEOA	Pt (3 wt%)	H₂	4.12 × 10³	4.84% λ = 420 nm	28 h	the crystalline honeycomb-like structures having high surface areas	[118]
BpCo-COF-1	λ ≥ 420 nm	AgNO₃	Co(NO₃)₂	O₂	152	0.46% λ = 420 nm	9 h	the coordinated Co²⁺as co-photocatalyst	[226]
TP-PN COF	λ > 420 nm	TEOA	Pt (12 wt%)	H₂	10,890	1.49% λ = 420 nm	24 h	shorten the linkage length	[338]
TP-BPyN COF					6457	1.80% λ = 420 nm		introduce nitrogen atoms
TP-BPyN PCOF					12,276	2.42%% λ = 420 nm		post-protonation

Fig. 28. (a) Synthesis of sp2c-Py-BT COF and imine-Py-BT COF and schematic chemical structures. (b) Photocatalytic overall water-splitting activity of different COFs. (c) AQE of sp2c-Py-BT COF at different wavelengths. (d,e) Calculated free energy diagrams of H2 production pathways on different active sites and water oxidation. (f) The full water dissociation pathways on the sp2c-Py-BT COF. Reprinted with permission from Ref. [317]. Copyright 2024, Wiley. (g) Top view (left), side view (middle) and partial enlarged detail (right) of AA stacking mode for Py-ClTP-BT-CO. (h) The photocatalytic activity of Py-XTP-BT-COFs. (i) Free-energy schemas for H2 evolution via a single-site reaction pathway at 0 V vs. RHE on the halogen substituted carbon of Py-XTP-BT-COFs. (j) The proposed H2 evolution reaction pathway on the halogen substituted carbon of Py-XTP-BT-COFs. Reprinted with permission from Ref. [314]. Copyright 2020, Wiley.

Fig. 29. (a) Top and side views of the AA stacked model of SQ-COF-1. (b) HRTEM images of SQ-COF-1. (c) Time-dependent photocatalytic degradation of SM2 curve. (d) The corresponding plots of ?ln(C/C0) vs. time for the SM2 degradation of the as synthesized samples. (e) ESR signals of the DMPO-?O2-. (f) Schematic diagram of the energy band structure for SQ-COF-1. Reprinted with permission from Ref. [256]. Copyright 2022, Wiley. (g) TEM image of Fe3O4@TpMa nanocomposite. (h) Photodegradation performance of phenol over different photocatalytic systems. (i) Pseudo-first-order kinetic fitting curves. (j) ESR signals for the DMPO-?OH. (k) Schematic of the degradation mechanism of Fe3O4@TpMa, and the process of ROS production in the Vis/Fe3O4@TpMa PMS system. Reprinted with permission from Ref. [339]. Copyright 2023, Wiley.

Table 2 COF-based photocatalysts applied in photocatalytic CO2 reduction.

Photocatalyst	Light source	Sacrificial agent	Photosensitizer	Product	Yield (μmol g^-1 h^-1)	Stability (h)	Characteristic	Ref.
TCOF-MnMo6	300W Xe lamp (800 > λ > 400 nm)	none	none	CO	36.2	20	highly conjugated π-electron structure	[366]
Co-TAPT-COF-1	300W Xe lamp (λ ≥ 420 nm)	TEOA	[Ru(bpy)₃]Cl₂	CO	8.39 × 10³	20	Co-N₂O₂ and Co-N₂O₂-Co-N₂O₂ coordination structure	[367]
CdS@COF	Xe lamp (λ ≥ 420 nm)	BIH	none	CO	507	10	CdS@COF core-shell structure	[368]
30%Ni-BDNs	300W Xe lamp (λ > 420 nm)	TEOA	[Ru(bpy)₃]Cl₂	CO	158.4 × 10³	15	strong interaction exists between the N/O component and the Ni component	[364]
PDA-TTA	300W Xe lamp (420 nm ≤ λ ≤ 800 nm)	CH₃CN /TEOA	none	HCOOH	65.7	40	the roles of triazine units on photocatalysis	[369]
TMBen-Perylene	λ > 420 nm	TEOA	none	CO	93	10	type-II heterostructure	[157]
Cu-SA/CTF	300 W Xe lamp (λ ≥ 420 nm)	TEA	none	CH₄	32.56	16	Cu-N-C₂ coordination structure	[370]
Co-2,3-DHTA-COF	λ ≥ 420 nm	TEOA	[Ru(bpy)₃]Cl₂	CO	18 × 10³	12	Co-O₄ active sites	[371]
Ru/TpPa-1	300W Xe lamp (800≥ λ ≥ 420 nm)	TEOA	none	HCOOH	108.8	20	The introduction of Ru NPs	[372]
sp²c-COF_dpy-Co	300W Xe lamp (λ > 420 nm)	TEOA	none	CO	1000	50	fully C=C bridged COFs containing metal ions	[373]
FDH@COFV2-Rh	λ = 420 nm	TEOA	none	HCOOH	1.46 × 10³	12	the collaborative matching of linkages and linkers	[312]
Ni-TpBpy	300 W Xe lamp (λ ≥ 420 nm)	TEOA	[Ru(bpy)₃]Cl₂	CO	966	6	the collaborative effects of single Ni catalytic site as well as TpBpy supporter	[374]
Re-COF	225W Xe lamp (λ > 420 nm)	TEOA	none	CO	~0.75 × 10³	9	Re(bpy)(CO)₃Cl postsynthetic modification	[375]
CoNi-COF-3	300W Xe lamp (λ > 420 nm)	TEOA	[Ru(bpy)₃]Cl₂	CO	2567	10	Co/Ni dual sites	[365]
pNJU-319Fe	300W Xe lamp (λ > 420 nm)	TEOA	none	CO	688	50	postsynthetic annulation	[224]

Fig. 30. (a) TEM image of Ni-BDNs. (b) Time-resolved CO and H2 production over 30%Ni-BDNs. (c) Wavelength dependence of CO and H2 evolution rate and light absorption spectrum of 30%Ni-BDNs. (d) In situ ATR-FTIR spectra of 30%Ni-BDNs. (e) Free-energy schemas for CO2 conversation to CO on 30%Ni-BDNs and 30%Ni-BD. Reprinted with permission from Ref. [364]. Copyright 2024, Wiley. (f) TEM image of CoNi-COF-3. (g) Control experiments over the CoNi-COF-3 photocatalyst. (h) AQE of CoNi-COF-3 at different wavelengths. In situ DRIFTS measurements for photocatalytic CO2 reduction over CoNi-COF-3 in the dark (0?20 min) (i) and under illumination (20?60 min) (j). (k) Free energy diagram of photocatalytic CO2 reduction to CO on the metal centers of Co-COF-3, Ni-COF-3, and CoNi-COF-3. Reprinted with permission from Ref. [365]. Copyright 2023, American Chemical Society.

Fig. 31. (a) SEM image of TpBD-(CH3)2. (b) Kinetic profiles of photocatalytic benzylamine oxidation by different COFs. (c) Aerobic oxidation of anilines with different substituents on TpTAB produces the corresponding imines. (d) Benzylamine conversion under different conditions over TpTAB. (e) Possible mechanism of photothermally catalyzed aniline oxidation on TpTAB. Reprinted with permission from Ref. [376]. Copyright 2023, American Chemical Society. (f) Top and side views; (g) HRTEM image of COF-JLU22. (h) Recycling photoreductive dehalogenation test of phenacyl bromide. (i) Schematic energy band structure of g-C3N4 and COF-JLU22. (j) Possible photoreductive dehalogenation reaction mechanism of COF-JLU22. Reprinted with permission from Ref. [377]. Copyright 2019, Elsevier.

Fig. 32. (a) TEM image (scale bar, 50 nm, inset, top view of COF1) of COF1. (b) Aberration-corrected HAADF-STEM image (scale bar, 2 nm) of COF1-Au (single Au atoms are indicated by red circles.). (c) NH3 production rates of different catalysts. (d) NH3 production rates of COF1-Au with different mass loadings of Au. (e) Proposed mechanism of photocatalytic nitrogen fixation over COFX-Au. Reprinted with permission from Ref. [378]. Copyright 2023, American Chemical Society. (f) SEM image of JLNU-303. (g) PHE curves. (h) Schematic energy bands of 3D-TTF-COFs. (i) Possible photocatalytic nitrogen fixation mechanism of 3D-TTF-COFs. (j) Free energy diagrams for NRR on 3D-TTF-COFs along the most favorable pathway. Reprinted with permission from Ref. [379]. Copyright 2024, Elsevier.

Fig. 33. (a) HRTEM and FFT images of EO-COF. (b) H2O2 photoproduction performance for EX-COFs. (c) EPR signals of DMPO-*O2- for EX-COFs. (d,e) Band alignment diagram and Schematic free energy diagram of EX-COFs. (f) Key steps of reaction pathways of H2O2 production by EO-COF. Reprinted with permission from Ref. [199]. Copyright 2024, Wiley. (g) HRTEM image of TPB-COF-OH. (h) Photocatalytic H2O2 yield rates for TPE-COF-OH, TPB-COF-OH, TPP-COF-OH, and TPB-COF-OMe. (i) UV-vis DRS spectrum and AQY comparison of TPB-COF-OH. (j) Free energy diagrams of TPB-COF-OH for the photosynthesis of H2O2 through the phenolic quinone transformation pathway and nonphenolic quinone transformation pathway. (k) Proposed reaction mechanism toward H2O2 production on the catechol moiety. Reprinted with permission from Ref. [380]. Copyright 2024, American Chemical Society.

Table 3 COF-based photocatalysts applied in photocatalytic H2O2 generation.

Photocatalyst	Light source	Solvent system	Yield (μmol g^-1 h^-1)	AQE (or AQY)	SCC	Stability	Characteristic	Ref.
TaptBtt	300W Xe lamp (λ > 420 nm)	water	1407	4.6% λ = 450nm	0.296%	96 h	spatially separated redox centers	[381]
SO₃H-COF	300W Xe lamp (λ > 400 nm)	H₂O/MeOH (9:1)	4971	15% λ = 400 nm	0.4%	5 h	polar oxygen-containing functional groups	[245]
EO-COF	300W Xe lamp (λ > 400 nm)	water/ethanol (9:1)	2675	6.57% λ = 450 nm	none	15 h	interconnected with VIA group elements	[199]
COF-LZU1	λ > 420 nm	water	387	none	none	10 h/24 h	autooxidation to Wurster's salt mimics	[382]
MPc-THHI-COFs (M=2H, Ni)	300W Xe lamp (λ > 400 nm)	water	4511/4589	none	none	four cycles	unprecedented noninterpenetrated shp topology	[119]
PMCR-1	300W Xe lamp (λ > 420 nm)	water/BA (10:1)	5500	14% λ = 420 nm	none	60 h	strong π-π interaction of BA and dangling phenyl moieties within the COF pores	[305]
TPB-COF-OH	300W Xe lamp (λ > 420 nm)	water	6608	9.61% λ = 420 nm	0.84%	12 h	integration of the redox-active catechol moiety into a series of COFs	[380]
TiCOF-spn	300W Xe lamp (780 ≥ λ ≥ 420 nm)	water/ethanol (9:1)	489.94	none	none	25 h	3D titanium COF with spn topology	[267]
ZT-5	Solar simulator (λ ≥ 360 nm)	water/ethanol (9:1)	2443	13.12% λ = 365 nm	none	4 h	S-scheme heterojunction between ZnO and TpPa-Cl	[280]
Bpy-TAPT	300W Xe lamp (λ > 420 nm)	H₂O	4038	8.6% λ = 420 nm	0.65 %	25 h	dual active sites (bipyridine and triazine)	[383]

Fig. 34. Challenges of COF-based photocatalysts.

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基于共价有机框架的光催化剂的研究进展: 原理、设计和应用

Recent advances of covalent organic frameworks-based photocatalysts: Principles, designs, and applications

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