导电金属有机框架材料在电催化中的成就，挑战和机遇

doi:10.3866/PKU.WHXB202010025

Abstract

Abstract:

To fulfill the demands of green and sustainable energy, the production of novel catalysts for different energy conversion processes is critical. Owing to the intriguing advantages of the intrinsic active species, tunable crystal structure, remarkable chemical and physical properties, and good stability, metal-organic frameworks (MOFs) have been extensively investigated in various electrochemical energy conversions, such as the CO₂ reduction reaction, N₂ reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and oxygen reduction reaction. More importantly, it is feasible to change the chemical environments, pore sizes, and porosity of MOFs, which will theoretically facilitate the diffusion of reactants across the open porous networks, thereby improving the electrocatalytic performance. However, owing to the high energy barriers of charge transfer and limited free charge carriers, most MOFs show poor electrical conductivity, thus limiting their diverse applications. As reported previously, MOFs were used as a porous substrate to confine the growth of nanoparticles or co-doped electrocatalysts after annealing. The conductive MOFs can combine the advantages of conventional MOFs with electronic conductivity, which significantly enhance the electrocatalytic performance. In addition, conductive MOFs can achieve conductivity via electronic or ionic routes without post-annealing treatment, thereby extending their potential applications. Different synthesis strategies have recently been developed to endow MOFs with electrical conductivity, such as post-synthesis modification, guest molecule introduction, and composite formatting. The performance of conductive MOFs can even outperform those of commercial RuO₂ catalysts or Pt-group catalysts. However, it is difficult to endow most MOFs with high conductivity. This review summarizes the mechanisms of constructing conductive MOFs, such as redox hopping, through-bond pathways, through-space pathways, extended conjugation, and guest-promoted transport. Synthetic methods, including hydro/solvothermal synthesis and interface-assisted synthesis, are introduced. Recent advances in the use of conductive MOFs as heterogeneous catalysts in electrocatalysis have been comprehensively elucidated. It has been reported that conductive MOFs can demonstrate considerable catalytic activity, selectivity, and stability in different electrochemical reactions, revealing the immense potential for future displacement of Pt-group catalysts. Finally, the challenges and opportunities of conductive MOFs in electrocatalysis are discussed. Based on systematic synthesis strategies, more conductive MOFs can be constructed for electrocatalytic reactions. In addition, the morphology and structure of conductive MOFs, which can change the electrochemical accessibility between substrates and MOFs, are also crucial for catalysis, and thus, they should be extensively studied in the future. It is believed that a breakthrough for high-performance conductive MOF-based electrocatalysts could be achieved.

Key words: Conductive metal-organic frameworks, Electrocatalysis, CO2 reduction reaction, N2 reduction reaction, Oxygen evolution reaction, Hydrogen evolution reaction, Oxygen reduction reaction

MSC2000:

O643

Zengqiang Gao, Congyong Wang, Junjun Li, Yating Zhu, Zhicheng Zhang, Wenping Hu. Conductive Metal-Organic Frameworks for Electrocatalysis:Achievements, Challenges, and Opportunities[J].Acta Phys. -Chim. Sin., 2021, 37(7): 2010025.

Figures/Tables 11

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Type	Catalyst	Electrolyte	Potential	FE	Ref.
CO₂RR	Fe_MOF-525 films	1.0 mol·L^-1 TBAPF₆ + 1 mol·L^-1 TFE	-1.3 V vs. NHE	∼100% (CO + H₂)	77
	HKUST-1 (Cu, Ru)	0.5 mol·L^-1 KHCO₃	-1.0 V vs. Ag/AgCl	47.2% (alcohol)	80
	Al₂(OH)₂TCPP-Co	0.5 mol·L^-1 potassium carbonate	-0.7 V vs. RHE	76% (CO)	82
	Ag@Al-PMOFs	0.1 mol·L^-1 KHCO₃	-1.1 V vs. RHE	55.8% (CO)	83
	Cu₂(CuTCPP)	0.5 mol·L^-1 EMIMBF₄	-1.55 V vs. Ag/Ag⁺	68.4% (formate); 16.8% (acetate)	84
	bismuthine (Bi-ene)	1 mol·L^-1 KOH	-0.57V vs. RHE	99.8% (formate)	85
ORR	Ni₃(HITP)₂	0.1 mol·L^-1 KOH	∼0.75 V vs. RHE	63% (H₂O₂)	27
	(Co)PCN222	0.1 mol·L^-1 HClO₄	0.43V vs. RHE		94
NRR	Mo₃(HAB)₂		0.18 V		107
	Co₃(HHTP)₂	0.5 mol·L^-1 LiClO₄	–0.40 V vs. RHE	3.34%	108
OER	{Fe₃(μ₃-O)(bdc)₃}₄{Co₂(na)₄(L^T)₂}₃	water at pH = 13	225 mV		112
	Fe/Ni-BTC	0.1 mol·L^-1 KOH	270 mV	95%	113
	NiCo-UMOFNs	1.0 mol·L^-1 KOH	∼189 mV	99.3%	114
	MAF-X27-OH(Cu)	1.0 mol·L^-1 KOH	292 mV	100%	115
	NiFe-NFF	1.0 mol·L^-1 KOH	227 mV	~100%	116
	NiFe MOF/OM-NFH	1.0 mol·L^-1 KOH	270 mV		117
HER	NiFe-MOF	0.1 mol·L^-1 KOH	240 mV		98
	Pd@MOF-74	0.5 mol·L^-1 H₂SO₄	-0.106 V vs. RHE		99
	Ni₃(Ni₃·HAHATN)₂	0.1 mol·L^-1 KOH	115 mV		100

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Conductive Metal-Organic Frameworks for Electrocatalysis:Achievements, Challenges, and Opportunities

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