Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduc-tion of[Cr(C2O4)3]3-into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr3+in[Cr(C2O4)3]3-,the intercalation of[Cr(C2O4)3]3-is expected to result in an electron-rich struc-ture of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C2O4)3]3--LDHs with more active Ni3+species and the expedited dynamic generation of Ni3+(Fe)OOH phase during the OER process con-tributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic struc-ture of metal sites,NiFe-[Cr(C2O4)3]3--LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm-2.This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni3+sites with the optimal electronic environment for improved OER electrocatalysis.

Yujie Wu;Minglei Song;Yu-Cheng Huang;Chung-Li Dong;Yingying Li;Yuxuan Lu;Bo Zhou;Dongdong Wang;Jianfeng Jia;Shuangyin Wang;Yanyong Wang

State Key Laboratory of Chemo/Bio-Sensing and Chemometrics,College of Chemistry and Chemical Engineering,the National Supercomputing Center in Changsha,Hunan University,Changsha 410082,Hunan,China;Department of Physics,Tamkang University,New Taipei City 25137,Taiwan,China;Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education),School of Chemistry and Material Science,Shanxi Normal University,Taiyuan 030031,Shanxi,China

能源化学

[1]Yujie Wu;Minglei Song;Yu-Cheng Huang;Chung-Li Dong;Yingying Li;Yuxuan Lu;Bo Zhou;Dongdong Wang;Jianfeng Jia;Shuangyin Wang;Yanyong Wang-.Promoting surface reconstruction of NiFe layered double hydroxides via intercalating[Cr(C2O4)3]3-for enhanced oxygen evolution)[J].能源化学,2022(11):140-148

Cr3+in,Ni3+species,Ni3+sites

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