Manipulating the structure self-reconstruction of transition metal sulfide-based(pre)catalysts during the oxygen evolution reaction(OER)process is of great interest for developing cost-effective OER catalysts,which remains a central challenge.Here we realize a deep structure self-reconstruction of natural chal-copyrite to unlock its OER performance via mechanochemical activation.Compared with the manually milled counterpart(CuFeS2-HM),the mechanically milled catalyst(CuFeS2-BM)with a reduced crys-tallinity exhibits a 7.11 times higher OER activity at 1.53 V vs.RHE.In addition,the CuFeS2-BM requires a low overpotential of 243 mV for generating 10 mA cm-2 and exhibits good stability over 24 h.Further investigations suggest that the excellent OER performance of CuFeS2-BM mainly originates from the decreased crystallinity induced the in situ deep structure self-reconstruction of the originally sulfides into the electroactive and stable metal(oxy)hydroxide phase(e.g.,α-FeOOH)via S etching under OER conditions.This study demonstrates that regulating the crystallinity of catalysts is a promising design strategy for developing highly efficient OER catalysts via managing the structure self-reconstruction pro-cess,which can be further extended to the design of efficient catalysts for other advanced energy conver-sion devices.In addition,this study unveils the great potentials of engineering abundant natural minerals as cost-effective catalysts for diverse applications.

Zhijie Chen;Renji Zheng;Wenfei Wei;Wei Wei;Bing-Jie Ni;Hong Chen

Centre for Technology in Water and Wastewater,School of Civil and Environmental Engineering,University of Technology Sydney,NSW 2007,Australia;State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control,Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials(SKLISEM),School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen 518055,Guangdong,China

能源化学

[1]Zhijie Chen;Renji Zheng;Wenfei Wei;Wei Wei;Bing-Jie Ni;Hong Chen-.Unlocking the electrocatalytic activity of natural chalcopyrite using mechanochemistry)[J].能源化学,2022(05):275-283

mechanochemistry,copyrite,tallinity

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