多核金属有机框架材料在电催化中的研究进展

doi:10.1016/S1872-2067(25)64859-5

催化学报 ›› 2026, Vol. 80: 59-91.DOI: 10.1016/S1872-2067(25)64859-5

多核金属有机框架材料在电催化中的研究进展

肖丽媛, 王振旅, 管景奇()

吉林大学化学学院, 物理化学研究所, 吉林长春 130021

收稿日期:2025-05-12 接受日期:2025-07-11 出版日期:2026-01-05 发布日期:2026-01-05
通讯作者: 管景奇
基金资助:
国家自然科学基金(22075099);吉林省自然科学基金(20220101051JC)

Advances in multinuclear metal-organic frameworks for electrocatalysis

Liyuan Xiao, Zhenlu Wang, Jingqi Guan()

Institute of Physical Chemistry, College of Chemistry, Jilin University, Changchun 130021, Jilin, China

Received:2025-05-12 Accepted:2025-07-11 Online:2026-01-05 Published:2026-01-05
Contact: Jingqi Guan
About author:Jingqi Guan (Jilin University) was invited as a young member of the 6th Editorial Board of Chin. J. Catal. and the 5th Editorial Board of Acta Phys.-chim. Sin. Prof. Jingqi Guan received his B.A. degree in 2002 and Ph.D. degree in 2007 from Jilin University. He carried out postdoctoral research in the University of California at Berkeley from 2012 to 2013 and in the Dalian Institute of Chemical Physics from 2014 to 2018. His research interests are in engineering single-atom catalysts and 2D materials for electrocatalysis, energy, and the environment. He has published more than 250 peer-reviewed papers.
Supported by:
National Natural Science Foundation of China(22075099);Natural Science Foundation of Jilin Province(20220101051JC)

摘要/Abstract

摘要：

金属有机框架材料(MOFs)因其高比表面积、可调孔径结构和多功能性, 在电催化领域展现出广阔的应用前景. 然而, 传统MOFs多采用单核金属离子构建, 存在活性位点有限、电子传输效率低等问题, 限制了其催化性能的进一步提升. 多核MOFs通过引入金属团簇作为次级构筑单元, 不仅显著增加了反应活性位点, 还赋予材料复杂的电子结构与稳定的几何构型, 展现出更优的电催化性能和调控潜力. 尽管相关研究日益增多, 但系统性总结仍较缺乏, 尤其在催化机制与结构调控策略方面尚缺少深入探讨.

本文围绕多核MOFs在电催化领域中的研究进展进行系统综述, 内容涵盖合成策略、表征方法、催化机制、性能调控及电催化应用五个方面. 首先, 归纳了原位组装与预组装两类构建方式, 并分析了合成过程中金属团簇结构调控的关键影响因素, 包括反应条件、配体类型及辅助试剂等. 其次, 介绍了多种原位表征技术(如红外光谱、拉曼光谱、X射线吸收精细结构、X射线光电子能谱等)在多核MOFs研究中的应用, 探讨它们对金属中心价态变化、配位环境演化和中间体形成过程的实时监测作用, 并分析其优缺点. 系统总结了多核MOFs在析氢、析氧、氧还原、CO₂还原、氮还原以及硝酸盐还原等典型电催化反应中的应用进展与催化作用机制. 在此基础上, 重点探讨了其在电催化过程中的作用本质. 多核金属团簇结构中金属位点间的协同作用、电子耦合以及构型调节可有效优化反应物的吸附与活化路径, 促进电子传输, 并稳定关键中间体, 从而显著提升催化性能与反应选择性. 此外, 重点讨论了多核MOFs的性能调控策略. 通过调节金属簇的核数、组成、电子结构及引入缺陷位点, 可实现对催化活性和选择性的精准调控; 同时, 通过配体功能化及活性位点微环境的调控, 也能进一步优化催化过程中的动力学行为与电子输运效率. 这些调控手段在不同反应体系中均展现出显著的性能提升效果. 最后, 指出当前多核MOFs在规模化制备、结构稳定性和真实活性位点识别方面仍面临挑战. 未来研究应加强构效关系的深入解析, 发展高通量筛选与多模态原位表征技术, 并推动多核MOFs材料向器件集成与工程化方向转化.

综上, 本文综述了多核MOFs的可控合成、原位表征、反应机制、调制策略和电催化应用, 并着重讨论了吸附、活性位点和电子转移在电催化过程中的作用. 该论文为多核MOFs的设计与应用提供了系统参考, 推动其在清洁能源催化体系中的应用进程.

关键词: 多核金属位点, 金属有机框架, 二氧化碳还原反应, 氧还原反应, 氮还原反应

Abstract:

Metal-organic frameworks (MOFs) with mononuclear metal ion nodes have garnered significant attention in the electrocatalytic field owing to their high surface area and tunable structures, but their development is critically hindered by the limitation of active site availability. In contrast, multinuclear MOFs exhibit notable advantages by offering multi-metal active sites, constructing complex structures, enhancing structural and thermal stability, and coupling with in-depth studies on catalytic mechanisms, endowing them great application potential in complex multi-electron reactions. This work provides a comprehensive review on the precise construction, in-situ characterizations, reaction mechanisms, modulation strategies, and electrocatalytic applications of multinuclear MOFs, underlying their role in electrocatalytic processes with a focus on adsorption, active sites, and electron transfer. The effects of spin, polarization, orbital coupling, and pore confinement on catalytic performance are systematically elucidated. Furthermore, the unique tuning strategies of multinuclear MOFs are summarized to guide the precise construction, including adjusting the type and number of metal cores, optimizing electronic structures, and manipulating defects. Lastly, the future trends in the development of multinuclear MOFs for electrocatalysis are envisioned, laying a solid foundation for their practical applications.

Key words: Multinuclear metal sites, Metal-organic framework, Carbon dioxide reduction reaction, Oxygen reduction reaction, Nitrogen reduction reaction

肖丽媛, 王振旅, 管景奇. 多核金属有机框架材料在电催化中的研究进展[J]. 催化学报, 2026, 80: 59-91.

Liyuan Xiao, Zhenlu Wang, Jingqi Guan. Advances in multinuclear metal-organic frameworks for electrocatalysis[J]. Chinese Journal of Catalysis, 2026, 80: 59-91.

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图/表 23

Fig. 1. (a) The development of MOFs. Reproduced with permission: Copyright 1997, Wiley‐VCH [24]; Copyright 2002, American Chemical Society [25]; Copyright 2004, Wiley‐VCH [26]; Copyright 2005, Elsevier Ltd. [27]; Copyright 2006, American Chemical Society[28]; Copyright 2008, American Chemical Society [29]; Copyright 2013, American Chemical Society [30]; Copyright 2014, American Chemical Society [31]; Copyright 2015, Wiley‐VCH [32]; Copyright 2017, Royal Society of Chemistry [33]; Copyright 2019, Royal Society of Chemistry [34]; Copyright 2022, Royal Society of Chemistry [35]. (b) The formation mechanism of MOFs. (c) Binuclear Ce-based MOF. Reproduced with permission [12]. Copyright 2022, American Chemical Society. (d) A trinuclear MOF. Reproduced with permission [36]. Copyright 2024, Wiley‐VCH. (e) Hexanuclear Zr-based MOF. Reproduced with permission [37]. Copyright 2022, Elsevier Ltd. (f) A dodecanuclear MOF. Reproduced with permission [38]. Copyright 2020, Wiley‐VCH.

Fig. 2. (a?f) Summary of synthesis methodologies of MOFs. Reproduced with permission [87]. Copyright 2024, Elsevier Ltd. Reproduced with permission [91]. Copyright 2022, Royal Society of Chemistry. Reproduced with permission [94]. Copyright 2022, Elsevier Ltd. Reproduced with permission [96]. Copyright 2024, Elsevier Ltd. Reproduced with permission [97]. Copyright 2023, Royal Society of Chemistry. Reproduced with permission [100]. Copyright 2022, Elsevier Ltd.

Table 1 Classification of multinuclear MOFs by SBU types.

SBU type	Nuclearity	Configuration	Representative MOFs	Ref.
Paddlewheel dinuclear cluster	2	quasi-square planar or distorted tetrahedral	HKUST-1 MOF-505	[44-47]
Trinuclear cluster	3	planar triangular	MIL-100(Fe) PCN-333	[48-51]
Tetranuclear cluster	4	tetrahedral	UiO-66 MIL-125(Ti)	[52-54]
Hexanuclear cluster	6	octahedral	UiO-67/68 MOF-808	[55-57]
High-nuclearity cluster	≥6	cube-like	ZJU-28 NU-1000	[58-61]
Dodecanuclear cluster	12	cage-like or wheel-like	Ln₁₂	[62]
Helical trinuclear chain	3	1D infinite chain	MIL-118	[63,64]
Wheel-shaped Mo cluster	6	cyclic wheel-shaped configuration	POMOFs Ni₈Mo₈	[65,66]
Defective Zr cluster	6-8	open octahedral configuration	DUT-67 MOF-545	[67,68]

Table 2 Classification of multinuclear MOFs by linkers.

Linker	Ligand	Structural characteristics	Coordination characteristics	Examples
Rigid dicarboxylic acid	terephthalic acid(H₂BDC), naphthalic acid (H₂NDC), anthraquinone diformic acid (H₂AQDC)	rigid main chain structure, π conjugation	multidentate, bridging ability	BIPT-3 [69] MCF-37 [70]
Flexible dicarboxylic acid	1,4-cyclohexanedicarboxylic acid (H₂CHDC), glutaric acid, Adipic acid	conformational flexibility, rotatable	high coordinative freedom, asymmetric topology	Cu₂(CHDC)₂ [71] [Zn(BTA)(chdc)_0.5]_n [72]
Tricarboxylic acid	trimesic acid (H₃BTC), trimellitic acid	multi-dimensional porous structure	multisite bridging, complex topological structures	HKUST-1 [73,74] TCNQ@Cu₃(BTC)₂[75] HKUST-1 [73,74]
Tetracarboxylic acid	pyromellitic acid (H₄BTEC)	high connectivity, high adaptability	polynuclear polymeric metal clusters, highly cross-linked 3D network structure	CTH-14 [76] Mg₅(OH)₂(BTEC)₂(H₂O)₄·11H₂O [77]
Pyrazolate	3,5-dimethylpyrazole (DMPZ), 1H-pyrazole-3,5-dicarboxylic acid (H₃PDC)	bearing a five-membered nitrogen heterocycle	π conjugatio, chelating or bridging	FDM-91 [78]
Imidazole	2-methylimidazole (2-MeIM), imidazole-4,5-dicarboxylic acid (H₃IDC)	high thermal and chemical stability	N-donor ligand, extended π-conjugation	ZIF-8 [79,80], ZIF-67 [81,82]
Phosphate	phenylphosphonic acid (PPA), aminomethylphosphonic acid (AMPA)	contains P=O and P-OH bonds, highly acidic multidentate oxygen donor	multidentate and multibridging, high coordination strength	Zr-MOFs/F-ssDNA [83]
N-heterocyclic carboxylic acids	pyridine-2,6-dicarboxylic acid (H₂PDC), imidazolecarboxylic acid	bearing N-heterocycles and carboxyl groups	N,O-multidentate coordination, assembly of multinuclear metal clusters	IHEP-11 [84]

Fig. 3. (a) The structure of MIL-100(Fe). Reproduced with permission [104]. Copyright 2017, American Chemical Society. (b) The coordination model of Ce-AQ. (c) Oxygen bridge groups of Ce-O-Ce in Ce-AQ. Reproduced with permission [12]. Copyright 2022, American Chemical Society. Structures of [RE3(μ3-OH)(COO)6] SBUs (d), RE-BDC (e) and RE-NDC (f). Reproduced with permission [105]. Copyright 2017, Royal Society of Chemistry.

Table 3 Comparison of in-situ vs. pre-assembled cluster approaches in constructing multinuclear MOFs.

Characteristic	In-situ by self-assembly	Pre-synthesize metal clusters
Representative example	MIL-100 (Fe) [103] Ce-AQ [12] UiO-66(Zr) [106] ZIF-8@XLPEO [107]	RE-BDC [105] PCN-242(Fe₂Co) [108] UiO-66-NH₂ [109]
Synthesis yield	relatively low yield, condition-dependent	relatively high yield; well-controlled assembly process
Crystallinity	relatively low crystallinity, unstable crystal quality	highly crystalline with uniform crystal quality
Controllability	poor control over nuclearity and morphology	precise control; uniform structure
Functional tunability	dynamic structure, uneven active site distribution	stable structure, well-defined active sites
Advantages	simple synthesis, diverse cluster structures	high controllability, facilitates functional design
Challenges	low reproducibility, low yield	complex synthesis, stringent conditions

Fig. 4. Common characterization methods and their characteristics.

Fig. 5. (a) In-situ IR cell. (b) In-situ Raman cell. (c) In-situ XRD cell. (d) In-situ XPS cell. (e) In-situ XAS cell. (f) In-situ cell for M?ssbauer measurements. Reproduced with permission [110]. Copyright 2024, American Chemical Society. (g) In-situ IR insight into the CO2 transfer process on CuSiF6-TPPY surface. Reproduced with permission [116]. Copyright 2024, Elsevier Ltd. (h) In-situ Raman exploration of CO2 adsorption and activation. Reproduced with permission [121]. Copyright 2022, American Chemical Society. In-situ XANES (i) and FE-EXAFS (j) at the Cu K-edge. Reproduced with permission [134]. Copyright 2022, American Chemical Society.

Fig. 6. (a) The mechanism for the HER in acid and alkaline electrolytes. Reproduced with permission [156]. Copyright 2021, Royal Society of Chemistry. (b) The Volcano plot of exchange current density as a function of ?GH*. Reproduced with permission[157]. Copyright 2019, Elsevier Ltd. Al 2p (c) and Ru 2p (d) spectra of Al0.35/Ru0.15-TCPP-CNTs, Al0.35/Ru0.15-TCPP and Al-TCPP. The charge density redistributions of the Al-TCPP (e), Al0.35/Ru0.15-TCPP (f) and Al0.35/Ru0.15-TCPP-CNTs (g) systems. (g) The feasible HER mechanism for the Al0.35/Ru0.15-TCPP-CNTs. (h) The feasible HER mechanism for the Al0.35/Ru0.15-TCPP-CNTs. Reproduced with permission [160]. Copyright 2024, Royal Society of Chemistry.

Table 4 Performance comparison of multinuclear MOFs for the HER.

Catalyst	η₁₀(mV)	Tafel slope (mV dec^‒1)	Electrolyte	Ref.
MOF-3	196	112.1	1.0 mol L^‒1 KOH	[165]
MOF-4	238	137.8	1.0 mol L^‒1 KOH	[165]
Co/Cu-MOF(3)	391	94	1.0 mol L^‒1 KOH	[159]
Al_0.35/Ru_0.15-TCPP	55	76.0	1.0 mol L^‒1 KOH	[160]
Mg₂V-MOF	195	174	1.0 mol L^‒1 KOH	[166]
Ni₁Fe₂-MOF@GC	373	107	0.1 mol L^‒1 KOH	[147]
Fe₂Zn-MOF	221	174	0.1 mol L^‒1 KOH	[167]
[Co_0.5(DIB)(HSA)](C₁₀H₈)0.5	135	84	1.0 mol L^‒1 KOH	[168]
[Co(DIB)_0.5(SA)]	294	96	1.0 mol L^‒1 KOH	[168]
[Co(DIB)_0.5(SA)]·(DIB)_0.5	349	121	1.0 mol L^‒1 KOH	[168]
Co₂Ni₁N	102.6	60.17	1.0 mol L^‒1 KOH	[169]
Co₃N	246.0	108.6	1.0 mol L^‒1 KOH	[169]
Ni₃N	296.1	133.2	1.0 mol L^‒1 KOH	[169]
[(Ce(HTCPP))·H₂O]_n	244	265	1.0 mol L^‒1 KOH	[170]

Fig. 7. (a) The proposed OER mechanismin in acid and alkaline electrolytes. Reproduced with permission [156]. Copyright 2021, Royal Society of Chemistry. Electron-transfer (b) process and (c) pathways in traditional AEM route. Electron-transfer pathways (d) and process in traditional LOM route (e). Reproduced with permission [176]. Copyright 2022, Wiley‐VCH. (f) Schematic illustration of OPM. Reproduced with permission [180]. Copyright 2024, American Chemical Society. (g) High-solution XPS spectra of Fe 2p in Fe2V-MOF and Fe3-MOF. (h) Schematic representation of the electronic coupling between V and Fe in Fe2V-MOF and Fe3-MOF. Reproduced with permission [166]. Copyright 2022, American Chemical Society. (i) EPR spectra. (j) DOS of Co 3d orbital. Reproduced with permission [182]. Copyright 2019, American Chemical Society.

Table 5 Performance comparison of multinuclear MOFs for the OER.

Catalyst	η₁₀ (mV)	Tafel slope (mV·dec^-1)	Electrolyte	Ref.
MOF-3	180	189.7	1.0 mol L^‒1 KOH	[165]
MOF-4	228	290.6	1.0 mol L^‒1 KOH	[165]
Co₄-Co-MOF	357	—	1.0 mol L^‒1 KOH	[40]
Co/Cu-MOF(1)	320	49	1.0 mol L^‒1 KOH	[159]
CUMSs-ZIF-67	320	53.7	1.0 mol L^‒1 KOH	[186]
BUT-124(Co)-S80	393	—	1.0 mol L^‒1 KOH	[181]
Fe₂V-MOF	314	58	1.0 mol L^‒1 KOH	[166]
Ni₁Fe₂-MOF@GC	283	41	0.1 mol L^‒1 KOH	[147]
Fe₂Co-MOF	339	36.2	1 mol L^‒1 KOH	[167]
Ni-MOF-Fe-Se-400	242	51.2	1 mol L^‒1 KOH	[187]
PCN-Fe₂Co-Fe₂Ni	271	67.7	1 mol L^‒1 KOH	[182]
[Co(dpda)(4,4′-bpy)]_n	448	93.3	1 mol L^‒1 KOH	[188]
AB&Ni-MOF(1:1)/GC	379	77	1 mol L^‒1 KOH	[189]
NNU-22	376	77.2	0.1 mol L^‒1 KOH	[190]
NNU-23	365	81.8	0.1 mol L^‒1 KOH	[190]
NiFe-NFF	227	38.9	1 mol L^‒1 KOH	[191]
Fe₂Ni MOF/NF	222	42.4	1.0 mol L^‒1 KOH	[192]
hov-IrO_x/CeO₂	251	55	0.1 mol L^‒1 HClO₄	[193]
FeNiBTC/SSM5	223.7	74.5	1 mol L^‒1 KOH	[194]
NiCoFeO_x@C-400	253	83.3	1 mol L^‒1 KOH	[195]

Fig. 8. The ORR pathways with AM (a) and DM (b) in acid and alkaline media. Reproduced with permission [199]. Copyright 2024, Royal Society of Chemistry. (c) The synthesis of Co4-M-MOFs (M = Cu, Co, and Zn). Reproduced with permission [40]. Copyright 2024, Wiley‐VCH. Volcano plots of the hydrogen adsorption free energy of HER with the PDOS at the Fermi level (d) and the calculated overpotentials of OER with the d-band positions (e). Reproduced with permission [147]. Copyright 2021, Royal Society of Chemistry.

Fig. 9. (a) Reaction pathways of the CO2RR. Reproduced with permission [213]. Copyright 2024, Elsevier Ltd. (b) The synthesis and structure of Cu-X. (c) Average FEs of HER and total CO2RR. (d) Average FEs of various reduction products over Cu-I. (e) PDOS of Cu atoms in Cu-Cl, Cu-Br, and Cu-I. (f) Intermediates among process of CO2 electroreduction on Cu-I. Reproduced with permission [230]. Copyright 2022, Wiley‐VCH. (g) The cage structure in the Cu1Ni-BDP MOF. XANES (h) and EXAFS (i) spectra. (j) Time-resolved in-situ XRD patterns. (k) In-situ ATR-SEIRAS spectra. Reproduced with permission [232]. Copyright 2023, American Chemical Society. XPS spectra of In 3d (l) and Mg 2p (m). (n) EPR spectrum. Reproduced with permission [233]. Copyright 2024, American Chemical Society. (o) FE at different operation voltages. (p) The distribution of unpaired electrons in InCo-ABDBC-HIN. Reproduced with permission [234]. Copyright 2023, Royal Society of Chemistry.

Table 6 Performance comparison of multinuclear MOFs for CO2RR.

Catalyst	Electrolyte	Product	Current density (mA cm^‒2)	FE (%)	Ref.
SNNU-42	0.5 mol L^‒1 H₂SO₄	HCOOH CO	77.2	91.3	[233]
Cu₁Ni-BDP	1.0 mol L^‒1 KOH	C₂H₄	278	52.7	[232]
InCo-ABDBC-HIN	0.5 mol L^‒1 EMIMBF₄	HCOOH CO	26	81.6	[234]
In-ABDBC-HIN	0.5 mol L^‒1 EMIMBF₄	HCOOH CO	25	79.97	[234]
In-ABDBC-HAIN	0.5 mol L^‒1 EMIMBF₄	HCOOH CO	19	71.94	[234]
C-Zn₁Ni₄ ZIF-8	0.5 mol L^‒1 KHCO₃	CO	71.5	98	[235]
(Me₂NH²⁺)[In^III-[Ni(C₂S₂(C₆H₄COO)₂)₂]]·3DMF·1.5H₂O	0.05 mol L^‒1 KHCO₃	HCOOH CO	36	91.47	[236]
MIL-68(In)-NH₂	0.1 mol L^‒1 KHCO₃	HCOOH	108	94.40	[237]
Cu-MOF-74	0.1 mol L^‒1 KHCO₃	CH₄	10.9	>50	[238]
Cu-I	1 mol L^‒1 KOH	CH₄	77.7	57.2	[230]
Cu dimer - HKUST-1	1 mol L^‒1 KOH	C₂H₄	262	45	[231]
3D-CTU-MCOF	0.5 mol L^‒1 EMIMBF₄	C₂	>20	26.4	[239]

Fig. 10. Schematic diagram of ENRR on the surface: dissociation mechanism (a), association distal mechanism (b), association alternating mechanism (c), and enzymatic mechanism (d). Reproduced with permission [243]. Copyright 2024, Elsevier Ltd. (e) Combined volcano diagrams for flat (black) and stepped (red) TM surfaces in N2 reduction via Heyrovsky reaction, without (solid) and with (dotted) H-bonds. Reproduced with permission [247]. Copyright 2012, Royal Society of Chemistry. (f) FEs and NH3 yields on the MIL-100 (Al). (g) NRR mechanism on the MIL-100 (Al). Reproduced with permission [42]. Copyright 2020, American Chemical Society.

Table 7 Performance comparison of multinuclear MOFs for NRR and NO3RR.

Catalyst	Electrolyte	Product	Yield	FE (%)	Ref.
MIL-100 (Al)	0.1 mol L^‒1 KOH	NH₃	10.6 μg h^-1 cm^-2 mg_cat.^-1	22.6	[42]
NH₂-MIL-88B-Fe	0.1 mol L^‒1 Na₂SO₄	NH₃	1.205 × 10^-10 mol s⁻¹ cm⁻²	5.66	[249]
MIL-88B-Fe	0.1 mol L^‒1 Na₂SO₄	NH₃	3.575 × 10^-11 mol s⁻¹ cm⁻²	5.59	[249]
MoP @PPC	0.1 mol L^‒1 HCl	NH₃	28.73 μg h^-1 cm^-2 mg_cat.^-1	2.48	[252]
Cu@Ce-MOF	0.1 mol L^‒1 KOH	NH₃	14.83 μg h^-1 cm^-2	10.81	[253]
Fe-TCPP	0.1 mol L^‒1 HCl	NH₃	44.77 μg h^-1 cm^-2 mg_cat.^-1	16.23	[254]
Co-TCPP	0.1 mol L^‒1 HCl	NH₃	28.3 μg h^-1 cm^-2 mg_cat.^-1	11.58	[254]
SO₃-MOF-808	0.5 mol L^‒1 Na₂SO₄	NH₃	97 μmol cm^-2 h	87.5	[251]
NiFeRu-MIL-53	1 mol L^‒1 KOH	NH₃	62.39 mg h^-1 cm^-2	100	[250]

Fig. 11. (a) The synthetic process of NiFeRu-MIL-53. Potential-dependent NH3 yield rate (b) and FENH3 (c) of NiFe-MIL-53 and NiFeRu-MIL-53. In-situ Raman spectra of NiFe-MIL-53 (d) and NiFeRu-MIL-53 (e). Reproduced with permission [250]. Copyright 2024, American Chemical Society. (f) The structure of SO3-MOF-808. (g) FE to ammonia, FE to nitrite, and selectivity toward ammonia. (h) Ammonia production rates. Reproduced with permission [251]. Copyright 2024, American Chemical Society.

Fig. 12. Reaction mechanisms of multinuclear MOFs in electrocatalysis.

Fig. 13. The ground state structure of Cr4, S = 3 spin state (a) and S = 13 spin state (b). Reproduced with permission [264]. Copyright 2016, American Chemical Society. (c) The electronic coupling between Fe and Ni in Fe2Ni-MIL-88B. Reproduced with permission [265]. Copyright 2021, Elsevier Ltd. Mechanism diagram of electron orbital coupling induced by interfacial BEF: free energy difference (d) and energy band diagram (e). Reproduced with permission [267]. Copyright 2024, Elsevier Ltd.

Fig. 14. (a) Structure diagrams of Fe2(DOBDC) and Fe2Cl2(BBTA). PDOS before (b) and after (c) Mo doping. (d) PDOS of Mo-*N1-N2 in *NN. (e) The charge transfer chain. Reproduced with permission [271]. Copyright 2022, American Chemical Society.

Fig. 15. Regulatory strategies of multinuclear MOFs in electrocatalysis.

Fig. 16. (a,b) FEs and corresponding NH3 yields. (c) Free energy diagram of electrocatalytic NO3RR pathway. Reproduced with permission [275]. Copyright 2024, American Chemical Society. (d) Visual representation of a V-shaped trinuclear cluster. (e) PDOS of the d orbitals of the catalytic active center. Reproduced with permission [147]. Copyright 2021, Royal Society of Chemistry. (f) The synthesis of Ni0.8Fe0.2-MOF-B. Reproduced with permission [278]. Copyright 2022, Wiley‐VCH. (g) 3D framework of Fe2M-MOF. Reproduced with permission [15]. Copyright 2023, Wiley‐VCH. (h) Coordination environment. Reproduced with permission [282]. Copyright 2024, American Chemical Society.

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多核金属有机框架材料在电催化中的研究进展

Advances in multinuclear metal-organic frameworks for electrocatalysis

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