首页|Engineering spin-dependent catalysts:chiral covalent organic frameworks with tunable electroactivity for electrochemical oxygen evolution

Engineering spin-dependent catalysts:chiral covalent organic frameworks with tunable electroactivity for electrochemical oxygen evolution

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The chiral-induced spin selectivity(CISS)effect offers promising prospects for spintronics,yet designing chiral materials that enable efficient spin-polarized electron transport remains challenging.Here,we report the utility of covalent organic frameworks(COFs)in manipulating electron spin for spin-dependent catalysis via CISS.This enables us to design and synthesize three three-dimensional chiral COFs(CCOFs)with tunable electroactivity and spin-electron conductivity through imine condensations of enantiopure 1,1'-binaphthol-derived tetraaldehyde and tetraamines derived from 1,4-benzenediamine,pyrene,or tetrathiafulvalene skeletons.The CISS effect of CCOFs is verified by magnetic conductive atomic force microscopy.Compared with their achiral analogs,these CCOFs serve as efficient spin filters,reducing the overpotential of oxygen evolution and improving the Tafel slope.Particularly,the diarylamine-based CCOF showed a low overpotential of430 mV(vs reversible hydrogen electrode)at 10 mA cm-2 with long-term stability comparable to the commercial RuO2.This enhanced spin-dependent OER activity stems from its excellent redox-activity,good electron conductivity and effective suppression effect on the formation of H2O2 byproducts.

3D chiral COFspin-dependent catalystsCISSelectrochemical oxygen evolution

Ziping Li、Yueyuan Xiao、Chao Jiang、Bang Hou、Yan Liu、Yong Cui

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School of Chemistry and Chemical Engineering,Frontiers Science Center for Transformative Molecules and State Key Laboratory of Metal Matrix Composites,Shanghai Jiao Tong University,Shanghai 200240,China

National Key R&D Program of ChinaNational Key R&D Program of ChinaNational Key R&D Program of ChinaNational Key R&D Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaKey Project of Basic Research of ShanghaiKey Project of Basic Research of ShanghaiShenzhen Science and Technology Program

2021YFA12004022022YFA15033022021YFA12003022021YFA1501501222251112233100721JC140170022JC1402000CJGJZD20210408091800002

2024

10.1093/nsr/nwae332

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ISSN：
年,卷(期)：2024.11(9)