非衍生金属有机框架纳米片电解水催化剂: 基础理论、调控策略和最新进展

doi:10.1016/S1872-2067(24)60153-1

催化学报 ›› 2024, Vol. 67: 21-53.DOI: 10.1016/S1872-2067(24)60153-1

非衍生金属有机框架纳米片电解水催化剂: 基础理论、调控策略和最新进展

郭英杰^a^,^b, 李世龙^a^,^b, 王竞洋^b, 石磊^b(), 刘迪^a(), 赵慎龙^b^,^c()

^a中国矿业大学(北京)化学与环境工程学院, 北京 100083
^b中国科学院纳米系统与多级次制造重点实验室, 中国科学院纳米科学卓越创新中心,国家纳米科学中心, 北京 100190
^c中国科学院大学, 北京 101408

收稿日期:2024-07-02 接受日期:2024-09-24 出版日期:2024-11-30 发布日期:2024-11-30
通讯作者: 石磊,刘迪,赵慎龙
基金资助:
国家自然科学基金(22373027);中央高校基本研究经费(2023ZKPYHH05)

Non-derivatized metal-organic framework nanosheets for water electrolysis: Fundamentals, regulation strategies and recent advances

Yingjie Guo^a^,^b, Shilong Li^a^,^b, Wasihun Abebe^b, Jingyang Wang^b, Lei Shi^b(), Di Liu^a(), Shenlong Zhao^b^,^c()

^aSchool of Chemical & Environmental Engineering, China University of Mining and Technology (Beijing), Beijing 100083, China
^bCAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China
^cUniversity of Chinese Academy of Sciences, Beijing 101408, China

Received:2024-07-02 Accepted:2024-09-24 Online:2024-11-30 Published:2024-11-30
Contact: Lei Shi, Di Liu, Shenlong Zhao
About author:Lei Shi (National Center for Nanoscience and Technology) received his Ph.D. degree from Beijing University of Chemical Technology in 2022. Currently, He is a postdoctoral fellow in National Center for Nanoscience and Technology. His research interests focus on the MOF and COF-based nanomaterials for water electrolysis, electrochemical CO₂ reduction and small molecule electrooxidation.
Di Liu (China University of Mining and Technology (Beijing)) received her B.S. degree from Shandong University in 2011 and Ph.D. degree from Tsinghua University in 2016. She is currently an associate professor in China University of Mining and Technology (Beijing). Her current research is focused on the rational synthesis and mechanism exploration of perylene diimide (PDI)-based organic semiconductor materials for visible-light-driven photocatalysis and photoelectrocatalysis.
Shenlong Zhao (National Center for Nanoscience and Technology, Chinese Academy of Science) received his B.E. degree from Shandong University in 2011. He obtained his Ph.D. degree from the Harbin Institute of Technology and the National Center for Nanoscience and Technology in 2017. And then, he was a postdoctoral fellow in the University of New South Wales and a FH Loxton Research Fellow in the University of Sydney. Currently, He is a professor/principal investigator in National Center for Nanoscience and Technology. His research interests focus on the preparation and application of functional inorganic and organic carbon nanomaterials for energy conversion and storage.
Supported by:
National Natural Science Foundation of China(22373027);Fundamental Research Funds for the Central Universities(2023ZKPYHH05)

摘要/Abstract

摘要：

随着全球能源需求的增加和环境问题的日益严峻, 开发清洁可再生能源已成为全球可持续发展的核心任务. 电解水制氢是实现绿色氢能生产的重要途径之一, 而催化剂的效率直接决定了电解水的反应性能. 传统贵金属催化剂虽然表现出优异的催化活性, 但高昂的成本和资源稀缺性限制了其大规模应用. 金属有机框架(MOF)材料具有独特的可调控结构和丰富的活性位点, 成为替代贵金属催化剂的理想候选之一. 尤其是非衍生MOF纳米片(MOFNSs), 其二维结构具有较大的比表面积和更高的活性中心暴露率, 在电解水反应中展现出显著优势. 因此, 研究非衍生MOF纳米片的基础理论和调控策略, 对于推动高效、经济的电解水技术至关重要.

非衍生MOFNSs在电解水中的应用潜力巨大, 本文从机理研究、结构表征、调控策略和最新进展四个方面系统地总结了该领域的基础理论与研究成果. 在电解水反应机制方面, 非衍生MOFNSs具有明确的结构为机理研究提供了理想的研究平台. 为进一步理解MOFNSs的结构-活性关系, 各种表征技术被广泛应用. 结构表征涉及高分辨透射电子显微镜、X射线吸收精细结构等先进技术, 用于研究MOFNSs的晶体结构、活性位点分布及其在电催化反应过程中的结构演变. 通过这些技术, 研究者能够深入探讨材料的微观结构与宏观催化性能之间的关系, 揭示催化活性来源, 并实现对催化剂设计的反馈优化. 在调控策略方面, 总结了多种提升MOFNSs催化性能的有效手段, 包括金属节点调控、配体设计、缺陷工程、复合工程以及其他策略. 通过调节电荷转移路径和活性位点性质选择金属节点, 显著影响催化性能; 而通过引入不同功能基团调节MOF的电子结构和孔径设计配体, 提升了活性位点的暴露和电子传导性. 此外, 缺陷工程通过引入氧空位或金属空位, 创造了更多未配位的活性位点, 提高了反应物吸附和电荷转移效率. 复合材料的设计则通过将MOFNSs与其他功能材料结合, 增强材料整体催化活性和稳定性. 除了常见设计策略外, 近期还涌现出许多新兴的改进方法以提升其电催化性能. 同时, 结合二维材料、无定形材料等新兴领域的研究, 也为开发高效、稳定的电催化剂提供了新思路. 在最新进展中, 研究者开发了多种MOFNSs催化剂, 在电解水反应中表现出较好的性能. 通过高效合成方法制备的MOFNSs表现出显著降低的过电位和较好的长时间稳定性, 同时在析氧反应和析氢反应中表现出较强的双功能催化能力. 通过先进的催化剂设计和表征技术, 研究进一步揭示了MOFNSs的反应机理, 优化了其在水分解过程中的应用潜力. 整体而言, 非衍生MOFNSs在电解水方面具有广阔的应用前景.

综上, 本文的系统总结为未来高效MOFNSs催化剂的设计与开发提供了重要的理论与实践参考. 未来的研究需在大规模生产、工业电流密度下的稳定性, 以及酸性电解质和海水电解方面继续突破. 通过先进表征以及人工智能的助力, 非衍生MOFNSs将进一步被优化, 并推动电解水技术向更高效、可持续方向发展.

关键词: 金属有机框架纳米片, 电催化, 水分解, 析氧反应, 析氢反应

Abstract:

Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen. Currently, noble metal (e.g. Iridium, Ruthenium, Platinum)-based catalysts are most widely used for water splitting electrolysis. However, noble metal-based catalysts often suffer from multiple disadvantages, including high cost, low selectivity and poor durability. The emergence of metal-organic framework nanosheets (MOFNSs) attracts significant attention due to their unique advantages. Here, a concise, yet comprehensive and critical, review of recent advances in the field of MOFNSs is provided. This review explains the fundamental oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) catalytic mechanisms as well as key characterization techniques for the structure-activity relationship study are discussed. Moreover, it discusses efficient design strategies and the brief research advances of MOFNSs in HER, OER, and bifunctional electrocatalysis, along with some challenges and opportunities.

Key words: Metal-organic framework nanosheets, Electrocatalysis, Water splitting, Oxygen evolution reaction, Hydrogen evolution reaction

郭英杰, 李世龙, 王竞洋, 石磊, 刘迪, 赵慎龙. 非衍生金属有机框架纳米片电解水催化剂: 基础理论、调控策略和最新进展[J]. 催化学报, 2024, 67: 21-53.

Yingjie Guo, Shilong Li, Wasihun Abebe, Jingyang Wang, Lei Shi, Di Liu, Shenlong Zhao. Non-derivatized metal-organic framework nanosheets for water electrolysis: Fundamentals, regulation strategies and recent advances[J]. Chinese Journal of Catalysis, 2024, 67: 21-53.

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图/表 19

Fig. 1. Main progress of MOFNSs for water electrolysis. Reproduced with permission from Ref. [25]. Copyright 2015, American Chemical Society; Ref. [26]. Copyright 2016, Nature Publishing Group; Ref. [16]. Copyright 2017, Nature Publishing Group; Ref. [151]. Copyright 2018, Wiley-VCH; Ref. [130]. Copyright 2019, Wiley-VCH; Ref. [18]. Copyright 2020, Nature Publishing Group; Ref. [132]. Copyright 2021, Nature Publishing Group; Ref. [115]. Copyright 2022, Nature Publishing Group; Ref. [50]. Copyright 2023, Wiley-VCH.

Fig. 2. Schematic diagram of the OER reaction path proposed in the previous study in alkaline: (A) AEM; (B) LOM; (C) OPM. (D) Volmer-Tafel and Volmer-Heyrovsky mechanisms of HER in alkaline and acidic condition. (E) Volcano plot of exchange current density as a function of the DFT-calculated Gibb's free energy (ΔGH*) of the adsorbed atomic hydrogen on a pure metal. Reproduced with permission from Ref. [41]. Copyright 2018, Royal Society of Chemistry.

Fig. 3. (A) Schematic diagram of technical principle. Reproduced with permission from Ref. [48]. Copyright 2022, Multidisciplinary Digital Publishing Institute. (B) Single-atom contrast in the range Z = 1-103 obtained by simulations iDPC-STEM image. Reproduced with permission from Ref. [49]. Copyright 2016, Elsevier. (C) IDPC-STEM images and GPA of Ni-BDC. Reproduced with permission from Ref. [50]. Copyright 2023, Wiley-VCH. (D) Simultaneous detection of SAXS and WAXS. (E) GIWAXS of UiO-66 on UiO-67 heterostructures. Reproduced with permission from Ref. [53]. Copyright 2023, Wiley-VCH. SAXS (F) and EXAFS (G) characterization of NiCo-UMOFNs. Reproduced with permission from Ref. [26]. Copyright 2016, Nature Publishing Group. (H) Schematic illustration of electrocatalytic water splitting. Reproduced with permission from Ref. [33]. Copyright 2020, Royal Society of Chemistry. (I) Typical polarization curves for HER (left) and OER (right). Reproduced with permission from Ref. [54]. Copyright 2017, Wiley-VCH.

Fig. 4. (A) In situ probing map of various representative in situ techniques. Reproduced with permission from Ref. [73]. Copyright 2020, American Chemical Society. Schema of in-situ Raman spectroscopy (B), in-situ mass spectroscopy (C), in-situ X-ray absorption spectroscopy (D), and in-situ transmission electron microscopy (E). Reproduced with permission from Ref. [76]. Copyright 2020, Royal Society of Chemistry. (F) Enhancing the connection between computation and experiments in electrocatalysis. Reproduced with permission from Ref. [79]. Copyright 2022, Nature Publishing Group. (G) Information theoretic methods in DFT and applications to chemical problems. Reproduced with permission from Ref. [80]. Copyright 2020, Wiley-VCH.

Fig. 5. (A) Operando SR-FTIR measurements of 4.3%-MOF at different potentials. (B) FTIR signal at 1048 cm-1 and Ni4+/Ni2+ ratio versus potential during ORR and OER. Reproduced with permission from Ref. [81]. Copyright 2019, Nature Publishing Group. (C) In situ FTIR spectra of bulk CuBDC at 150 °C. Reproduced with permission from Ref. [82]. Copyright 2024, Wiley-VCH. (D) Electrochemical in situ Raman spectra of Ni0.9Fe0.1-MOF and Ni-MOF in the range of 350-700 cm−1 at operated potentials from 1.1 to 1.67 V vs. RHE. Reproduced with permission from Ref. [83]. Copyright 2022, Elsevier. (E) Ni K-edge Fourier-transformed k3-weighted EXAFS signals recorded at different potentials in 1 mol L-1 KOH. (F) comparison of Ni K-edge EXAFS WTs recorded for the pristine sample, standard references and catalytic materials at 1.1, 1.3 and 1.5?V. Reproduced with permission from Ref. [18]. Copyright 2020, Nature Publishing Group.

Fig. 6. (A) Different metal nodes in the MOF crystal structure. Reproduced with permission from Ref. [91]. Copyright 2021, Wiley-VCH. (B) Strategies to construct stable MOFs guided by HSAB theory. Reproduced with permission from Ref. [92]. Copyright 2018, Wiley-VCH.

Fig. 7. Synthesis (A), molecular and crystal structure schematic diagrams (B) and Co 2p XPS spectrum (C) of ultrathin 2D Co-MOF nanosheet catalysts. Reproduced with permission from Ref. [89]. Copyright 2018, Royal Society of Chemistry. (D) Synthesis. AFM (E) and S 2p XPS spectrum (F) of the 2DSP single-layer sheet. Reproduced with permission from Ref. [93]. Copyright 2015, Wiley-VCH. (G) Scheme of the cobalt dithiolene films. Reproduced with permission from Ref. [94]. Copyright 2015, American Chemical Society. (H) Schematic illustration, synthesis and photograph of the structure of the 2D coordination polymers. Reproduced with permission from Ref. [95]. Copyright 2017, American Chemical Society. (I) Surfactant-assisted phase-selective synthesis of new cobalt MOFs. Reproduced with permission from Ref. [96]. Copyright 2017, Wiley-VCH.

Fig. 8. Crystal structure (A) and AFM image (B) of NiCo-UMOFNs. (C) Schematic representation of the electronic coupling between Co and Ni in UMOFNs. Reproduced with permission from Ref. [26]. Copyright 2016, Nature Publishing Group. (D) Schematic illustration of the 2D oxide sacrifice approach conversion of M-ONS with 2,5-dihydroxyterephthalic acid to form M-MNS. Reproduced with permission from Ref. [90]. Copyright 2019, Wiley-VCH. (E) Comparison of the overpotentials required for 10 mA cm-2 for substituted M (M = Fe, Co, Cu, Mn, and Zn) in Ni-MOFs. Reproduced with permission from Ref. [98]. Copyright 2021, Wiley-VCH.

Fig. 9. (A) Formation process of FeCo2Ni-MOF-74 at ambient temperature. (B) Catalytical reaction circle and active sites for FeCo2Ni-MOF-74 with rich Ovac. (C) DOS for various materials. Reproduced with permission from Ref. [99]. Copyright 2021, Elsevier. (D) Schematic illustration of microwave-assisted synthesis of ultrathin trimetal-organic framework nanosheets, (Reproduced with permission from Ref. [100]. Copyright 2021, Elsevier. Synthetic process (E), HRTEM image (scale bar is 5 nm) (F) and AFM image and corresponding height profile (G) of the 2D HE-MOFs array. (H) The overpotential testing at a current density of 50 mA cm-2 of overall samples under 1.0 mol L-1 KOH. Reproduced with permission from Ref. [101]. Copyright 2022, American Chemical Society.

Fig. 10. (A) Schematic illustration of 2D Co-MOFs with different organic ligands. (B) Bader charge transfer and magnetic moments of Co sites in different 2D Co-MOFs. Reproduced with permission from Ref. [106]. Copyright 2023, American Chemical Society. (C) Structural modelling of FeNi-MOFs modulated by halogen atoms. (D) Calculated PDOS and Ni-3d band center. (E) Ni K-edge XANES spectra. Reproduced with permission from Ref. [107]. Copyright 2024, Wiley-VCH. (F) Schematic representation for the formation of the self-supporting 2D Ni-MOF nanosheet electrode. Reproduced with permission from Ref. [110]. Copyright 2022, American Chemical Society. (G) 2D planar structure of Ni-MOF. Reproduced with permission from Ref. [114]. Copyright 2023, American Chemical Society.

Fig. 11. (A) HRTEM (top) and SEM (bottom) images of the pristine 1.7%-, 3.6%- and 4.3%-MOFs. (B) Fourier transforms of the Ni K-edge EXAFS spectra. Reproduced with permission from Ref. [81]. Copyright 2019, Nature Publishing Group. (C) Schematic illustration of the NaBH4 defect post-treatment. (D) DOS and the corresponding structures (inset) of Co-MOF and Co-MOF-VO. (E) Charge density mapping at [010] facet. Reproduced with permission from Ref. [118]. Copyright 2020, Wiley-VCH. (F) Electronic structure of MOF is regulated by a missing linker. Reproduced with permission from Ref. [119]. Copyright 2020, Wiley-VCH. (G) Modulating electronic structure and DOS of MOFs via introducing missing linkers. Reproduced with permission from Ref. [120]. Copyright 2019, Nature Publishing Group.

Fig. 12. (A) Schematic illustration of the formation of flexible lattice matching junction in MOF-on-MOF epitaxy. Reproduced with permission from Ref. [124]. Copyright 2014, American Chemical Society. (B) A representation of the combinations of three distinctive processes of MOF-on-MOF growth. Reproduced with permission from Ref. [125]. Copyright 2020, Wiley-VCH. (C) Illustration of the Synthesis Process of the FePc@Ni-MOF composite nanosheets. Reproduced with permission from Ref. [128]. Copyright 2021, American Chemical Society. (D) Hierarchical Ni3S2@2D Co MOF nanosheets as efficient hetero-electrocatalyst for hydrogen evolution reaction in alkaline solution. Reproduced with permission from Ref. [129]. Copyright 2022, Elsevier. (E) Schematic of the synthesis process for Co-BDC/MoS2 hybrid nanosheets. Reproduced with permission from Ref. [130]. Copyright 2019, Wiley-VCH. (F) Schematic illustration for the preparation of NiRu0.13-BDC catalyst. Reproduced with permission from Ref. [132]. Copyright 2021, Nature Publishing Group.

Fig. 13. (A) Models of optimized NiBDC and S-NiBDC. (B) Structure of active site for [FeFe]-hydrogenase, (C) PDOS of p-states for NiBDC and S-NiBDC models. (D) Polarization curves of S-NiBDC and Pt/C. (E) FESEM images of S-NiBDC after HER tests at different current densities. (F) In-situ Raman spectra of S-NiBDC at −0.3 V vs. RHE for different times. (G) In-situ ATR-FTIR spectra of S-NiBDC with the potential of 0 to −0.4?V vs. RHE. (H) Polarization curves of S-NiBDC in 1.0 mol L-1 NaOH H2O solution and 1.0 mol L-1 NaOD D2O solution. Reproduced with permission from Ref. [135]. Copyright 2022, Nature Publishing Group.

Table 1 MOFNSs for electrocatalytic HER in recent years.

Number	Catalyst	η@10 mA cm^-2/mV	Tafel slope/mV dec⁻¹	Condition	Stability	Ref.
1	Ni₃(Ni₃·HAHATN)₂	115	45.6	0.1 mol L⁻¹ KOH	1000 cycles	[113]
2	Co MOF/H₂	30	88	1.0 mol L⁻¹ KOH	40 h@10 mA cm^-2	[140]
3	AB&CTGU-5	44	45	0.5 mol L⁻¹ H₂SO₄	96 h@10 mA cm^-2	[96]
4	[Cu(2,5-pydc)(H₂O)]n·2H₂O	340	70	1.0 mol L⁻¹ KOH	1000 cycles	[138]
5	NiFe-MOF-74	195	136	1.0 mol L⁻¹ KOH	5000 cycles	[141]
6	Ni₃S₂@2D Co-MOF/CP	140	90.3	1.0 mol L⁻¹ KOH	2000 cycles	[129]
7	THTNi 2DSP	333	80.5	0.5 mol L⁻¹ H₂SO₄	—	[93]
8	FePc@Ni-MOF	334	72.1	0.1 mol L⁻¹ KOH	10 h@10 mA cm^-2	[128]
9	Pt-NC/Ni-MOF	25	42.1	1.0 mol L⁻¹ KOH	10000 cycles	[142]
10	2D Ni-MOF@Pt	43	30	0.5 mol L⁻¹ H₂SO₄	—	[143]
11	MoS₂/Co-MOF-3	262	51	0.5 mol L⁻¹ H₂SO₄	25000 s@10 mA cm^-2	[137]
12	UiO-66-NH₂-Mo/GC	125	59	0.5 mol L⁻¹ H₂SO₄	5000 cycles	[144]
13	THTA-Co	283	71	0.5 mol L⁻¹ H₂SO₄	400 cycles	[145]
14	3ZIF-67-Pt/RGO	14.3	12.5	0.5 mol L⁻¹ H₂SO₄	1000 cycles	[146]
15	3ZIF-67-Pt/RGO	37.2	33.1	1.0 mol L⁻¹ KOH	1000 cycles	[146]
16	NiFe-MOF array	68	112	1.0 mol L⁻¹ KOH	22 h@~550 mA cm^-2	[103]
17	AB&Co-Cl₄-MOF(3:4)	283	86	1.0 mol L⁻¹ KOH	1000 cycles	[136]
18	NiRu-MOF/NF	51	90	1.0 mol L⁻¹ KOH	5000 cycles	[148]
19	D-Ni-MOF	101	50.9	1.0 mol L⁻¹ KOH	1000 cycles	[120]
20	Co-BDC/MoS₂	248	86	1.0 mol L⁻¹ KOH	2000 cycles	[130]
21	Fe(OH)_x@Cu-MOF	112	76	1.0 mol L⁻¹ KOH	30 h@10 mA cm^-2	[139]
22	Ce-MOF@Pt-0.05	208	188.1	1.0 mol L⁻¹ KOH	3,000 cycles	[149]
23	CoP/Co-MOF	52	44	0.5 mol L⁻¹ H₂SO₄	20 h@20 mA cm^-2	[131]
24	S-NiBDC	100	75	1.0 mol L⁻¹ KOH	150 h@1000 mA cm^-2	[135]
25	IF@CoFe-TDPAT NSA	212.2	76.7	1.0 mol L⁻¹ KOH	24 h@300 mA cm^-2	[147]

Fig. 14. (A) Illustration of the synthesis of bulk, 3D, and 2D MOFs. iR-corrected polarization curves for OER (B) and corresponding Tafel plots derived from the LSV curves (C). Reproduced with permission from Ref. [150]. Copyright 2021, Wiley-VCH. (D) Schematic illustration of the preparation of MOFNSs. (E) Coordination structure of CuBDC before and after thermal treatment and liquid nitrogen exfoliation. (F) SEM image of bulk CuBDC and 2D CuBDC after thermal treatment and liquid nitrogen exfoliation, Characterization of OER catalytic activity of different materials. Linear sweep voltametric curves and Tafel plots of bulk CuBDC and CuBDC-5 (G) and bulk NiBDC and NiBDC-5 (H). Reproduced with permission from Ref. [82]. Copyright 2024, Wiley-VCH.

Table 2 MOFNSs for electrocatalytic OER in recent years.

Number	Catalyst	η@10 mA cm^-2/mV	Tafel slope/mV dec⁻¹	Condition	Stability	Ref.
1	Co₃(HITP)₂	254	86.5	1.0 mol L^-1 KOH	12 h@16 mA cm^-2	[162]
2	NiCo-UMOFNs	250	42	1.0 mol L^-1 KOH	200 h@10 mA cm^-2	[26]
3	FeCo-MNS-1.0	298	21.6	0.1 mol L^-1 KOH	10000 s@~22 mA cm^-2	[90]
4	NiFe-MOF	215	49.1	1.0 mol L^-1 KOH	40 h@10 mA cm^-2	[98]
5	FeCo₂Ni-MOF-74	254	21.4	0.1 mol L^-1KOH	100 h@10 mA cm^-2	[99]
6	MW-Ni₄Co₄Fe₂-UMOFNs	243	48.1	1.0 mol L^-1 KOH	10 h@12 mA cm^-2	[100]
7	UNi-MOFNs-2	170	41	1.0 mol L^-1 KOH	3,000 cycles	[110]
8	NiFe-MOF NSs	240	73.44	1.0 mol L^-1 KOH	16 h@10 mA cm^-2	[111]
9	Fe:2D-Co-NS@Ni	211	46	0.1 mol L^-1 KOH	95 h@10 mA cm^-2	[86]
10	Ni-BPDC	415	83	1.0 mol L^-1 KOH	20000 s@5 mA cm^-2	[114]
11	Ni-MOF	370	101.9	0.1 mol L^-1 KOH	1000 cycles	[153]
12	Co-ZIF-9(III)	380	55	1.0 mol L^-1 KOH	10 h@15 mA cm^-2	[85]
13	Ni-Fe-MOF	221	56	1.0 mol L^-1 KOH	20 h@10 mA cm^-2	[154]
14	NiFe-UMNs	260	30	1.0 mol L^-1 KOH	10000 s@60 mA cm^-2	[155]
15	Ni-MOF@Fe-MOF	265	82	1.0 mol L^-1 KOH	—	[151]
16	2D CoFe-MOF	355	49.05	0.1 mol L^-1 KOH	15 h@20 mA cm^-2	[156]
17	CoFe MOFNSs	276	46.7	1.0 mol L^-1 KOH	—	[157]
18	CoFe-MOF-OH	265	44	1.0 mol L^-1 KOH	40 h@10 mA cm^-2	[158]
19	TMOF-4	318	54	1.0 mol L^-1 KOH	15 h@20 mA cm^-2	[159]
20	CoNi-MOF/rGO	318	48	1.0 mol L^-1 KOH	50 h@10 mA cm^-2	[160]
21	CoBDC-Fc_0.17	178	61	1.0 mol L^-1 KOH	80 h@100 mA cm^-2	[119]
22	CoNi(1:1)-MOF	265	56	1.0 mol L^-1 KOH	20 h@25 mA cm^-2	[161]
23	IF@CoFe-TDPAT NSA	226.4	30.8	1.0 mol L^-1 KOH	24 h@300 mA cm^-2	[147]

Fig. 15. (A) Schematic preparation of Ru@Cr-FeMOF. (B) Schematic diagram of the mechanism of the Cr-O-Ru interface regulating the orbitals of ruthenium nanoclusters. (C) LSV polarization curves with Ru@Cr-FeMOF||Ru@Cr-FeMOF electrodes and Pt/C||RuO2 electrodes. (D) Comparison of total water splitting performance between Ru@Cr-FeMOF and reported catalysts. Reproduced with permission from Ref. [152]. Copyright 2024, Wiley-VCH. (E) Schematic representation of synthesis procedure. (F) Voltages of water splitting electrolyzer at different current densities (10-500 mA cm−2). (G) J-V curves of silicon solar cell under simulated AM 1.5G 100 mW cm−2 illumination with water photolysis. Reproduced with permission from Ref. [103]. Copyright 2021, Elsevier.

Table 3 MOFNSs for electrocatalytic water splitting in recent years.

Number	Catalyst	ηOER@10 mA cm^-2/mV	ηHER@10 mA cm^-2/mV	Condition	Cell Voltage	Stability	Ref.
1	NiFe-MOF-74	208	195	1.0 mol L^-1 KOH	1.65 V@20 mA cm^-2	3000 cycles	[141]
2	D-Ni-MOF	219	101	1.0 mol L^-1 KOH	1.63 V@100 mA cm^-2	48 h@100 mA cm^-2	[120]
3	NiFe-MOF array	215	68	1.0 mol L^-1 KOH	1.87 V@500 mA cm^-2	30 h@~17 mA cm^-2	[103]
4	NiFe-MOF	240	134	0.1 mol L^-1 KOH	1.55 V@10 mA cm^-2	20 h@~12 mA cm^-2	[16]
5	CoNi(1:1)-MOF	265	120	1.0 mol L^-1 KOH	1.48 V@10 mA cm^-2	80000 s@20 mA cm^-2	[161]
6	BP@MOF	266	88	1.0 mol L^-1 KOH	1.63 V@10 mA cm^-2	10 h@12 mA cm^-2	[163]
7	Ni_0.3Co_0.7-9AC-AD	350	143	1.0 mol L^-1 KOH	1.56 V@10 mA cm^-2	30 h@~12 mA cm^-2	[164]
8	Ni₂V-MOFs@NF	244	89	1.0 mol L^-1 KOH	1.55 V@10 mA cm^-2	80 h@10 mA cm^-2	[165]
9	Ni@CoO@CoMOFC	247	138	1.0 mol L^-1 KOH	1.61 V@10 mA cm^-2	24 h@50 mA cm^-2	[166]
10	CoFe-PBA NS@NF-24	256	48	1.0 mol L^-1 KOH	1.545 V@10 mA cm^-2	36 h@100 mA cm^-2	[167]
11	NiFe-MS/MOF@NF	290	90	1.0 mol L^-1 KOH	1.61 V@10 mA cm^-2	27 h@50 mA cm^-2	[168]
12	NH₂-MIL-88B(Fe₂Ni)/NF	240	87	1.0 mol L^-1 KOH	1.56 V@10 mA cm^-2	30 h@500 mA cm^-2	[169]
13	Ru@Cr-FeMOF	190	21	1.0 mol L^-1 KOH	1.48 V@10 mA cm^-2	80000 s@20 mA cm^-2	[152]
14	IF@CoFe-TDPAT NSA	226.4	212.2	1.0 mol L^-1 KOH	1.43 V@10 mA cm^-2	100 h@300 mA cm^-2	[147]

Fig. 16. Several key challenges and prospects to enhance the performance of MOFNSs electrocatalysts and accelerate their application process.

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非衍生金属有机框架纳米片电解水催化剂: 基础理论、调控策略和最新进展

Non-derivatized metal-organic framework nanosheets for water electrolysis: Fundamentals, regulation strategies and recent advances

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