高效光催化金属有机框架(MOFs)的构筑策略

doi:10.1016/S1872-2067(23)64556-5

催化学报 ›› 2023, Vol. 55: 1-19.DOI: 10.1016/S1872-2067(23)64556-5

• 综述 • 下一篇

高效光催化金属有机框架(MOFs)的构筑策略

刘成^a, 刘胡润卿^a, 余济美^a^,^b, 吴棱^a^,^*(), 李朝辉^a^,^*()

^a福州大学化学学院, 能源与环境光催化国家重点实验室, 光催化研究所, 福建福州 350116
^b香港中文大学化学系, 香港新界

收稿日期:2023-09-12 接受日期:2023-10-31 出版日期:2023-12-18 发布日期:2023-12-07
通讯作者: *电子信箱: zhaohuili@fzu.edu.cn (李朝辉), wuling@fzu.edu.cn (吴棱).
基金资助:
国家自然科学基金(22372038);国家自然科学基金(22272026);“111计划”(D16008)

Strategies to engineer metal-organic frameworks for efficient photocatalysis

Cheng Liu^a, Hurunqing Liu^a, Jimmy C. Yu^a^,^b, Ling Wu^a^,^*(), Zhaohui Li^a^,^*()

^aResearch Institute of Photocatalysis, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, Fujian, China
^bDepartment of Chemistry, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong, China

Received:2023-09-12 Accepted:2023-10-31 Online:2023-12-18 Published:2023-12-07
Contact: *E-mail: zhaohuili@fzu.edu.cn (Z. Li), wuling@fzu.edu.cn (L. Wu).
About author:Ling Wu (State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University) received his Ph.D degree in 2004 from The Chinese University of Hong Kong. His research interests currently focus on photocatalysis and new materials based on MOFs and ultrathin inorganic metal oxide nanosheets, especially revealing the relationship of the surface structure and performances at molecular level. He has coauthored more than 260 peer-reviewed papers.
Zhaohui Li (State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University) received her Bachelor degree from Fudan University in 1990, Master degree from Fujian Institute of Research on Structure of Matter, Chinese Academy of Science in 1996, and PhD degree from National University of Singapore in 2000. She carried out postdoctoral research at University of Notre Dame (USA) from 2000 to 2002. She joined the faculty of Fuzhou University in 2003 and is currently a full professor of State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University. Her current research interest centers on the development of porous/nanostructured materials, in particular the MOFs materials, for photocatalytic applications, especially in photocatalytic organics transformations.
Supported by:
National Natural Science Foundation of China(22372038);National Natural Science Foundation of China(22272026);111 Project(D16008)

摘要/Abstract

摘要：

面对全球能源短缺和环境污染等问题, 发展绿色、可持续的能源来替代传统的化石能源成为迫切需求. 太阳能作为一种清洁可再生能源, 其有效转化与利用受到了广泛关注. 光催化将太阳能转化为化学能, 其核心是新型高效的光催化材料. 金属有机框架材料(MOFs), 是一类由金属或金属节点与多齿有机配体相互连接而成的微介孔材料, 具有独特的组成结构和特性, 有望成为有应用前景的光催化材料. 目前已有一些关于MOFs基光催化的综述, 但考虑到该领域在过去几年迅速发展, 为了研发高效的MOFs基光催化材料, 非常有必要对已经报道的用于提高MOFs基光催化剂性能的策略进行总结.

本综述重点总结了已报道的通过调控MOFs基材料的组成和结构的策略来提升其光催化性能的最新研究进展. 首先, 简要介绍了MOFs基材料的结构特点及其在光催化领域应用的优势, 阐述了MOFs基材料光催化的基本原理, 提出了影响其光催化性能的关键因素, 包括光吸收能力、光生载流子的分离和迁移以及催化活性位点. 其次, 阐明不同结构调控策略通过优化关键因素进而提高光催化性能的原理, 具体包括MOFs基材料中金属掺杂、配体功能化、超薄二维材料构筑以及缺陷工程策略. 然后, 通过总结典型案例, 详细讨论了上述策略如何通过调控MOFs基材料的组成和结构来优化关键因素, 从而提高MOFs基材料的光催化性能. 最后, 针对MOFs基材料光催化所面临的机遇、挑战及其发展趋势提出展望: (1) 影响MOFs基光催化剂效率的因素是多方面的, 因此将不同策略相结合有利于更好地提高MOFs基光催化剂的性能. 除了本文总结的四种构筑策略, 最近其它一些关于提升MOFs基材料光催化性能的结构调控策略也有零星报道, 如微环境调控、晶面工程等, 也值得进一步关注. (2) 与无机半导体光催化剂相比, MOFs基材料的结构稳定性较差, 因此应特别注意其在光催化条件下的稳定性, 特别是MOFs基材料在水中的反应体系. (3) 先进原位表征技术的发展和理论研究的深化对于高效MOF基光催化系统的设计及机理研究至关重要. (4) MOFs基材料的多功能性可以使其作为光诱导一锅多步反应的多功能催化材料, 应大力开展研究.

综上, 本文系统地总结了通过调控MOFs基材料的组成和结构从而达到提升其光催化性能的不同策略, 并就MOFs基材料光催化所面临的机遇、挑战及其发展趋势提出展望. 希望本文能够为深入了解MOFs基光催化体系中组成-结构-性能关系以及从原子水平来设计研发高效的MOFs基光催化剂提供参考.

关键词: 金属有机框架, 光催化, 金属掺杂, 配体功能化, 超薄二维MOFs, 缺陷工程

Abstract:

Photocatalysis, a promising technology to convert solar energy to chemical energy, is expected to relieve the global energy shortage and environmental pollution and therefore has attracted widespread recent research attention. Metal-organic frameworks (MOFs), a class of micro-mesoporous hybrid material constructed from metal or metal nodes interconnected with multi-dentated organic linkers, have recently been demonstrated to be promising photocatalysts for a variety of reactions relevant to environmental and energy concerns due to their unique structure and characteristics. Considering that MOF-based photocatalysis burgeoned rapidly during the past several years, and with an aim to develop more efficient MOF-based photocatalytic materials, it is still necessary to summarize the strategies already reported to improve the performance of MOF-based photocatalytic materials, even though several excellent reviews on MOF-based photocatalysis have already been published. In this review, four structural engineering strategies to improve the efficiency of MOF-based photocatalysis have been summarized. These strategies include metal doping, ligand functionalization, the fabrication of ultrathin 2D MOFs, and defect engineering. These methods aim to enhance light absorption, improve charge separation and transportation, and create more catalytic active sites. Personal opinions on the opportunities, challenges, and developing trends of MOF-based photocatalysis were addressed. This review aims to provide guidance for the rational development of advanced MOF-based photocatalysts by elucidating the inherent relationship between their structural properties and catalytic activity.

Key words: Metal-organic framework, Photocatalysis, Metal doping, Ligand functionalization, Ultrathin 2D MOFs, Defect engineering

刘成, 刘胡润卿, 余济美, 吴棱, 李朝辉. 高效光催化金属有机框架(MOFs)的构筑策略[J]. 催化学报, 2023, 55: 1-19.

Cheng Liu, Hurunqing Liu, Jimmy C. Yu, Ling Wu, Zhaohui Li. Strategies to engineer metal-organic frameworks for efficient photocatalysis[J]. Chinese Journal of Catalysis, 2023, 55: 1-19.

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图/表 18

Fig. 1. Concept of MOFs by interconnecting metal ions/clusters with multi-dentated organic ligands to form a crystalline network via the coordination bonds.

Fig. 5. (a) TEM image and corresponding EDS elemental mapping images of MIL-100(Fe0.63Al0.37). Reprinted with permission from Ref. [61]. Copyright 2022, Elsevier. (b) The mechanism of NNU-31-M CO2RR with H2O oxidation. The free-energy profile for the CO2RR pathway (c) and OER pathway (d). Reprinted with permission from Ref. [62]. Copyright 2019, Wiley-VCH. (e) Schematic illustration of synthetic of the PCN-250-Fe3 and PCN-250-Fe2M (Mn, Zn, Ni, Co) by Fe3 or Fe2M and H4abtc. (f) Comparison of photocatalytic activity of PCN-250-Fe3 and PCN-250-Fe2M for CO evolution. Reprinted with permission from Ref. [69]. Copyright 2020, Elsevier.

Table 1 Summary of metal doped MOF-based photocatalytic systems.

No.	MOFs	Method	Application	Ref.
1	Cu-doped NH₂-MIL-125(Ti)	Cu(NO₃)₂ + Ti(OC₄H₉)₄ + NH₂-BDC, 150 °C, 24 h	pollutant degradation	[57]
2	Fe-doped NH₂-MIL-68(In)	In(NO₃)₃ + Fe(NO₃)₃ + NH₂-BDC, 125 °C, 5 h	pollutant degradation	[65]
3	V-doped NH₂-MIL-125(Ti)	VCl₃ + Ti(OCH(CH₃)₂)₄ + NH₂-BDC, 120 °C, 72 h	none	[56]
4	Nb-doped NH₂-UiO-66(Zr)	NbCl₅ + ZrCl₄ + NH₂-BDC, 120 °C, 48 h	none	[56]
5	Ti-doped NH₂-UiO-66(Zr)	NH₂-UiO-66(Zr) + TiCl₄(THF)₂, 100 °C for 4 d	CO₂ reduction, H₂ evolution	[58,59]
6	Hf-doped-SH-UiO-66(Zr)	ZrCl₄ + HfCl₄ + 2SH-BDC, 120 °C, 48 h	N₂ fixation	[66]
7	Ce/Ti-doped UiO-66(Zr)	UiO-66(Zr/Ce) + TiCl₄(THF)₂, 120 °C, 4 d	H₂ evolution, O₂ evolution	[67]
8	Ni-doepd NH₂-MIL-125(Ti)	Ni(NO₃)₂ + Ti(OC₄H₉)₄ + NH₂-BDC, 150 °C, 20 h	CO₂ reduction	[68]
9	Al-doped MIL-100(Fe)	AlCl₃ + FeCl₃ + 1,3,5-benzene tricarboxylate, 150 °C, 36 h	organic syntheses	[61]
10	Co, Ni, Zn-doped NNU-31-M	Fe₂M(Co, Ni, Zn) cluster + TCA, 150 °C, 32 h	CO₂ reduction coupled with H₂O oxidation	[62]
11	Mn, Zn, Ni, Co-doped PCN-250-Fe₃	Fe₂M (Mn, Zn, Ni, Co) + H₄abtc, 140 °C, 2 h	CO₂ reduction	[69]
12	Co-doped Cu-MOF	Cu(NO₃)₂ + Co(NO₃)₂+ TCPP, 80 °C, 24 h	N₂ fixation	[70]

Fig. 6. (a) UV-vis spectra of MIL-125(Ti) (a) and NH2-MIL-125(Ti) (b). (b) Proposed mechanism for the photocatalytic CO2 reduction over NH2-MIL-125(Ti) under visible light irradiation. Reprinted with permission from Ref. [75]. Copyright 2012, Wiley-VCH. Frontier electron density of unsubstituted MIL-125: (c) the valence band is composed of the bdc C 2p orbitals, making these favorable for linker-based band gap modifications; (d) the conduction band is composed of O 2p orbitals and Ti 3d orbitals, suggesting that modifications of the aromatic bdc units are unlikely to affect the CB. Reprinted with permission from Ref. [73]. Copyright 2013, American Chemical Society.

Table 2 Absorption energies (Eabs, in eV) and ligand-to-metal charge-transfer energies (ELMCT, in eV) of UiO-66(Ce)-X. Reprinted with permission from Ref. [84]. Copyright 2018, American Chemical Society.

Energy	H	NH₂	NO₂	F	Cl	Br	I	OH	SH	COOH	CH₃	CF₃
E_abs	4.09	2.74	3.77	3.83	3.57	3.42	2.97	3.02	2.54	3.43	3.83	4.03
E_LMCT	-1.43	-1.57	-1.33	-1.38	-1.39	-1.42	-1.44	-1.61	-1.59	-1.65	-1.47	-1.35

Fig. 7. (a) Illustration showing the dark photocatalysis over MIL-125 and MIL-125 with different functional groups, MIL-125-X (X = NH2, NO2, Br). (b) Overlapping percentage and distance between electrons and holes in MIL-125 and MIL-125-X (X = NH2, NO2). Reprinted with permission from Ref. [87]. Copyright 2022, Royal Society of Chemistry. (c) Photocatalytic reduction of aqueous Cr(VI) over UiO-66-X (X = H, NH2, NO2 and Br) under simulated sunlight (320-780 nm). Reprinted with permission from Ref. [88]. Copyright 2015, Royal Society of Chemistry. Transient photocurrent response (d) and EIS Nyquist plots (e) of MIL-68(In)-X (X = H, NH2, NO2, Br). Reprinted with permission from Ref. [89]. Copyright 2018, Elsevier.

Fig. 8. (a) TEM image (scale bar: 500 nm). (b) AFM image and corresponding height profile. Reprinted with permission from Ref. [97]. Copyright 2018, Wiley-VCH. (c) Illustration for the synthesis of 2D Ln-TCPP nanosheets and the thickness- and metal-node-dependent photocatalytic activity. Reprinted with permission from Ref. [98]. Copyright 2020, Wiley-VCH. (d) Schematic of the synthesis process of Mn-TBAPy-BK (bulk) and Mn-TBAPy-NS (nanosheets) MOFs. (e) Photocatalytic H2 evolution activities of Mn-TBAPy-BK and Mn-TBAPy-NS before (left) and after (right) normalized to Pt content. Reprinted with permission from Ref. [104]. Copyright 2022, American Chemical Society.

Table 3 Summary of MOF-based photocatalytic systems obtained via ligand functionalization.

No.	MOFs	Method	Application	Ref.
1	NH₂-MIL-125(Ti)	Ti(OC₄H₉)₄+ NH₂-BDC, 150 °C, 72 h	CO₂ reduction	[75]
2	NH₂-MIL-125(Ti)	Ti(OC₃H₇)₄) + NH₂-BDC, 150 °C, 48 h	H₂ production	[76]
3	NH₂-MIL-125(Ti)	Ti(OC₄H₉)₄ + NH₂-BDC, 150 °C, 72 h	organic syntheses	[77]
4	NH₂-MIL-125(Ti)	Ti(OC₄H₉)₄ + NH₂-BDC, 150 °C, 72 h	N₂ fixation	[78]
5	OH/CH₃-MIL-125(Ti)	MIL-125(Ti) + OH-BDC/CH₃-BDC, 150 °C, 72 h	N₂ fixation	[78]
6	NH₂-UiO-66(Zr)	ZrCl₄ + NH₂-BDC, 120 °C, 48 h	H₂ production	[79]
7	NH₂-UiO-66(Zr)	ZrCl₄ + NH₂-BDC, 120 °C, 48 h	Organic syntheses	[80]
8	NH₂-UiO-66(Zr)	ZrCl₄ + NH₂-BDC, 120 °C, 48 h	Cr(VI) reduction	[81]
9	NH₂-UiO-66(Zr)	ZrCl₄ + NH₂-BDC, 120 °C, 48 h	CO₂ reduction	[82]
10	NH₂-MIL-101(Fe)	FeCl₃+ NH₂-BDC, 110 °C, 24 h	CO₂ reduction	[23]
11	NH₂-MIL-53(Fe)	FeCl₃ + NH₂-BDC, 150 °C, 72 h	CO₂ reduction	[23]
12	NH₂-MIL-88B(Fe)	FeCl₃+ NH₂-BDC, 170 °C, 24 h	CO₂ reduction	[23]
13	NH₂-MIL-88B(Fe)	FeCl₃+ NH₂-BDC, 150 °C, 15 min	Cr(VI) reduction	[83]
14	NH₂/(NH₂)₂-MIL-125(Ti)	Ti(OC₃H₇)₄) + NH₂BDC/(NH₂)₂-BDC, 150 °C, 48 h	none	[73]
15	NH₂-MIL-125(Ti)	Ti-(OC₃H₇)₄) + NH₂-BDC, 110 °C, 72 h	none	[86]
16	NH₂-125(Ti)	Ti(OC₄H₉)₄ + NH₂-BDC, 130 °C, 15 h	H₂ production	[87]
17	NO₂/Br-MIL-125(Ti)	MIL-125(Ti) + OH-BDC/CH₃-BDC, 130 °C, 15 h	H₂ production	[87]
18	NH₂/NO₂/Br-UiO-66(Zr)	ZrCl₄ + NH₂-BDC/NO₂-BDC/Br-BDC, 120 °C, 48 h	Cr(VI) reduction	[88]
19	NH₂/NO₂/Br-MIL-68(In)	In(NO₃)₃ + NH₂-BDC/NO₂-BDC/Br-BDC, 125 °C, 5 h	Cr(VI) reduction	[89]
20	CH₃/NO₂/Br-UiO-66(Ce)	(NH₄)₂Ce(NO₃)₆ + CH₃-BDC/NO₂-BDC/Br-BDC, 100 °C, 15 min	organic syntheses	[90]

Fig. 9. (a) Illustration of the synthetic route towards Pt single-atom coordinated ultrathin MOF nanosheets (PtSA-MNSs) through a surfactant-stabilized coordination strategy for photocatalytic hydrogen production. Reprinted with permission from Ref. [105]. Copyright 2019, Wiley-VCH. (b) Schematic representation showing the one-pot synthesis of PCN-134-3D and stepwise synthesis of PCN-134-2D nanosheets with accessible catalytic sites. Reprinted with permission from Ref. [106]. Copyright 2019, Wiley-VCH. (c) TEM image of g-CNQDs/PMOF. (d) Proposed mechanism of CO2 reduction over g-CNQDs/PMOF hybrids under visible-light irradiation. Reprinted with permission from Ref. [107]. Copyright 2019, American Chemical Society.

Fig. 10. (a) The fs-TA spectra (pump at 400 nm) taken at several representative probe delays for UiO-66-NH2-0 and UiO-66-NH2-100. (b) fs-TA kinetics and the global fitting results (probing in the range 580-650 nm using 8 traces with a 10-nm interval) for UiO-66-NH2-X (X = 0, 50, 100, 150, 200). (c) Comparison of photocatalytic H2 production rates and average relaxation lifetimes. Reprinted with permission from Ref. [120]. Copyright 2019, Wiley-VCH.

Table 4 Summary of ultrathin 2D MOF-based photocatalytic systems.

No.	MOF nanosheet	Method	Application	Ref
1	Ni-BDC MOFs	Ni(NO₃)₂ + H₂BDC, 140 °C, 12 h, exfoliation	CO₂ reduction	[91]
2	ZIF-67(Co)	Co(NO₃)₂ + 2-methylimidazole, room temperature, 30 min	CO₂ reduction	[94]
3	Ni₃(HITP)₂ MOFs	NiCl₂ + HITP·HCl + NH₃·H₂O, 65 °C, 2 h, exfoliation	CO₂ reduction	[95]
4	Zr-porphyrinic (Ni-TCPP) MOF	ZrCl₄ + Ni-TCPP, 120 °C, 24 h	organic syntheses	[97]
5	Porphyrin-based Ln-MOF (Ln = Ce, Sm, Eu, Tb, Yb)	Ce(NO₃)₃/Sm(NO₃)₃/Sm(NO₃)₃/Yb(NO₃)₃+ HAc + H₂TCPP, 10 min, microwave	organic syntheses	[98]
6	Porphyrin-based Ti-MOF	Ti(OC₄H₉)₄ + H₂TCPP, 150 °C, 5 d	organic syntheses	[99]
7	NH₂-MIL-125(Ti)	Ti(OC₄H₉)₄ + NH₂-BDC, 120 °C, 12 h	CO₂ reduction	[100]
8	MOF-74(Ni)	Ni(CH₃COO)₂ + H₄DOBDC, 120 °C, 12 h	organic syntheses	[101]
9	[Co(Ni-H₇TPPP)₂]·8H₂O MOFs	Co(CH₃COO)₂ + Ni-H₈TPPP + HCl, exfoliation	CO₂ reduction	[102]
10	Co-MOF-Ru(tpyCOO)₂	Co(NO₃)₂ + [Ru^II(tpyCOOH)₂](PF₆)₂, 120 °C, 24 h, exfoliation	H₂ production	[103]
11	Mn-MOF	MnCl₂ + H₄TBAPy, 130 °C, 72 h, exfoliation	H₂production	[104]
12	Pt single atoms/porphyrin-based Cu-MOF	Cu(NO₃)₂ + PtTCPP, 80 °C, 4 h.	H₂production	[105]
13	Photosensitizers-anchored Zr-BTB MOF	Zr-BTB nanosheets + H₄TCPP, 100 °C for 12 h	organic syntheses	[106]
14	g-CNQDs//porphyrin-based Co-MOF	Co(NO₃)₂ + TCPP, 150 °C, 4 h.	CO₂ reduction	[107]

Fig. 12. (a) Illustration of the synthesis for defective NH2-MIL-125(Ti) via the thermal treatment. Reprinted with permission from Ref. [132]. Copyright 2021, Elsevier. (b) A plausible mechanism of linker elimination by the photothermal treatment in a water medium containing TEOA. Reprinted with permission from Ref. [133]. Copyright 2020, Elsevier. (c) Schematic illustration of the synthetic procedures for ZIF-67-MBI via SALE approach. Reprinted with permission from Ref. [135]. Copyright 2023, Elsevier.

Fig. 13. (a) Idealized process of generation of defects in UiO-66: missing linker defect and missing cluster defect. Reprinted with permission from Ref. [137]. Copyright 2017, Elsevier. (b) Illustration of the crystal structures of UiO-66-fresh, UiO-66-UV-vis, and UiO-66-PSE. Reprinted with permission from Ref. [138]. Copyright 2021, Royal Society of Chemistry. (c) Schematic illustration of varied defective structures. (d) Photoreduction CO2 to CO evolution rates over NH2-UiO-66(Zr) with different types of defects. Reprinted with permission from Ref. [139]. Copyright 2021, Elsevier.

Table 5 Summary of defect containing MOF-based photocatalytic systems.

No.	Defective MOFs	Method	Application	Ref.
1	NH₂-UiO-66(Zr)	modulation approach	H₂ production	[120]
2	Cu-BTC MOFs	mixed linker approach	H₂ production, O₂ production	[123]
3	ZIF-67(Co)	mixed linker approach	H₂ production	[124]
4	NH₂-MIL-125(Ti)	thermal treatment	Cr(VI) reduction	[132]
5	NH₂-MIL-125(Ti)	photo-thermal treatment	H₂ production	[133]
6	ZIF-67(Co)	SALE approach	H₂ production, O₂ production	[135]
7	UiO-66(Zr)	photo treatment, SALE approach	N₂ fixation	[128]
8	NH₂-MIL-125(Ti)	SALE approach	H₂production	[131]
9	MIL-125(Ti)	SALE approach	H₂O₂ production	[134]
10	NH₂-UiO-66(Zr)	modulation approach, thermal treatment	CO₂ reduction	[139]
11	(SH)₂-UiO-66(Zr)	thermal treatment	N₂ fixation	[116]

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高效光催化金属有机框架(MOFs)的构筑策略

Strategies to engineer metal-organic frameworks for efficient photocatalysis

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