Unlocking the electrocatalytic activity of natural chalcopyrite using mechanochemistry

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

作者机构：Centre for Technology in Water and WastewaterSchool of Civil and Environmental EngineeringUniversity of Technology SydneyNSW 2007Australia State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution ControlShenzhen Key Laboratory of Interfacial Science and Engineering of Materials(SKLISEM)School of Environmental Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055GuangdongChina 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2022年第31卷第5期

页      面：275-283页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：financially supported by the National Natural Science Foundation of China (21777045, 61875119) the Australian Research Council (ARC) Future Fellowship (FT160100195) the Foundation of Shenzhen Science Technology and Innovation Commission (SSTIC)(2020231312, JCYJ20190809144409460) the Natural Science Funds for Distinguished Young Scholar of Guangdong Province,China (2020B151502094) the China Scholarship Council (CSC) for the scholarship support 

主　　题：Mechanochemistry Crystallinity Oxygen evolution reaction Self-reconstruction Mineral electrocatalysts 

摘      要：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 chalcopyrite to unlock its OER performance via mechanochemical activation. Compared with the manually milled counterpart(CuFeS_(2)-HM), the mechanically milled catalyst(CuFeS_(2)-BM) with a reduced crystallinity exhibits a 7.11 times higher OER activity at 1.53 V vs. RHE. In addition, the CuFeS_(2)-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 CuFeS_(2)-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., a-Fe OOH) 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 process, which can be further extended to the design of efficient catalysts for other advanced energy conversion devices. In addition, this study unveils the great potentials of engineering abundant natural minerals as cost-effective catalysts for diverse applications.