Enhanced reconstruction of Fe_(5)Ni_(4)S_(8) by implanting pyrrolidone to unlock efficient oxygen evolution  

作　　者：Zhengyan Du Zeshuo Meng Chao Jiang Chenxu Zhang Yanan Cui Yaxin Li Chong Wang Xiaoying Hu Shansheng Yu Hongwei Tian 

机构地区：[1]Key Laboratory of Automobile Materials of MOE,School of Materials Science and Engineering,Jilin University,Changchun 130012,Jilin,China [2]College of Science and Laboratory of Materials Design and Quantum Simulation,Changchun University,Changchun 130022,Jilin,China

出　　处：《Journal of Energy Chemistry》2023年第9期112-121,共10页能源化学（英文版）

基　　金：financially supported by the Scientific and Technological Development Program of Jilin Province (20220201138GX)。

摘　　要：During oxygen evolution reaction(OER),complex changes have been reported on surfaces of bimetallic Fe-Ni-based catalysts,and regulating the dynamic evolution could improve their electrocatalytic performances.Herein,a pyrrolidone-promoted reconstruction of pentlandite was investigated to uncover the correlation between the reconstructed surface and the OER performance.The theoretical calculations indicated the preferential implantation of pyrrolidone at Fe atoms,useful for regulating the electronic structures of pentlandite.The vale nce state of Ni increased,suggesting the promotion of the in-situ reconstruction of pentlandite via strengthening hydroxyl adsorption to generate highly active NiOOH.The electron-rich pentlandite was also found conducive to charge transfer under applied voltages.The Operando Raman and various quasi-in-situ characterizations confirmed the realization of more delocalized electronic structures of pentlandite by introducing pyrrolidone.This,in turn,promoted the accumulation of hydroxyl groups on the pentlandite surface,thereby boosting the formation of highly active NiOOH at lower OER potentials.Consequently,the adsorption energies of intermediates were optimized,conducive to enhanced OER reaction kinetics.As a proof of concept,the pentlandite decorated by pyrrolidone exhibited an overpotential as low as 265 mV at 10 mA cm^(-2) coupled with stable catalysis for 1000 hours at a high current density of 100 mA cm^(-2).In sum,new insights into unlocking the high catalytic activity of bimetallic Fe-Ni-based catalysts were provided,promising for future synthesis of advanced catalysts.

关 键 词：PENTLANDITE Oxygen evolution reaction Reconstruction ability Catalytic kinetics 

分 类 号：TQ116.2[化学工程—无机化工] TQ426