期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202307832
关键词
Electrocatalysis; Heptacoordinated Fe-Complex; Hydrogen Energy; Ligand Effect; Water Splitting
In this research, highly efficient heterogeneous bifunctional electrocatalysts have been designed through Fe coordination complexes, which modify the Fe centre for the electrolysis of H2O. By replacing -Cl- with -SO42-, the modified complex exhibits superior bifunctional activity with low overpotential and small Tafel slope. Additionally, it also demonstrates high-performance alkaline electrolyzer and remarkable stability. Therefore, exploring the intrinsic properties of metal-organic framework-based ECs provides a new approach for the rational design of molecular catalysts.
In this research, highly efficient heterogeneous bifunctional (BF) electrocatalysts (ECs) have been strategically designed by Fe coordination (C-R) complexes, [Fe2L2(H2O)(2)Cl-2] (C1) and [Fe2L2(H2O)(2)(SO4)].2(CH4O) (C2) where the high seven C-R number synergistically modifies the electronic environment of the Fe centre for facilitation of H2O electrolysis. The electronic status of Fe and its adjacent atomic sites have been further modified by the replacement of -Cl- in C1 by -SO42- in C2. Interestingly, compared to C1, the O-S-O bridged C2 reveals superior BF activity with extremely low overpotential (& eta;) at 10 mA cm(-2) (140 mV(OER), 62 mV(HER)) and small Tafel slope (120.9 mV dec(OER)(-1), 45.8 mV dec(HER)(-1)). Additionally, C2 also facilitates a high-performance alkaline H2O electrolyzer with cell voltage of 1.54 V at 10 mA cm(-2) and exhibits remarkable long-term stability. Thus, exploration of the intrinsic properties of metal-organic framework (MOF)-based ECs opens up a new approach to the rational design of a wide range of molecular catalysts.
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