Tuning synergy between nickel and iron in Ruddlesden-Popper perovskites through controllable crystal dimensionalities towards enhanced oxygenevolving activity and stability  

作　　者：Haijuan Zhang Daqin Guan Yuxing Gu Hengyue Xu Chunchang Wang Zongping Shao Youmin Guo 

机构地区：[1]School of Materials Science and Technology,Anhui University,Hefei,Anhui,China [2]Department of Building and Real Estate,The Hong Kong Polytechnic University,Hung Hom,Hong Kong,China [3]WA School of Mines:Minerals,Energy and Chemical Engineering,Curtin University,Perth,Western Australia,Australia [4]State Key Laboratory of Materials-Oriented Chemical Engineering,Nanjing Tech University,Nanjing,Jiangsu,China [5]Tsinghua Shenzhen International Graduate School,Tsinghua University,Shenzhen,Guangdong,China

出　　处：《Carbon Energy》2024年第6期113-123,共11页碳能源（英文）

基　　金：Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2023A1515012878;Natural Science Foundation of Anhui Province,Grant/Award Number:2008085ME134;Australian Research Council Discovery Projects,Grant/Award Numbers:ARC DP200103315,ARC DP200103332;Major Special Science and Technology Project of Anhui Province,Grant/Award Number:202103a07020007;Key Research and Development Program of Anhui Province,Grant/Award Number:202104a05020057。

摘　　要：Ni-Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction(OER)in water electrolysis.However,understanding and mastering the synergy of Ni and Fe remain challenging.Herein,we report that the synergy between Ni and Fe can be tailored by crystal dimensionality of Ni,Fe-contained Ruddlesden-Popper(RP)-type perovskites(La_(0.125)Sr_(0.875))n+1(Ni_(0.25)Fe_(0.75))nO3n+1(n=1,2,3),where the material with n=3 shows the best OER performance in alkaline media.Soft X-ray absorption spectroscopy spectra before and after OER reveal that the material with n=3 shows enhanced Ni/Fe-O covalency to boost the electron transfer as compared to those with n=1 and n=2.Further experimental investigations demonstrate that the Fe ion is the active site and the Ni ion is the stable site in this system,where such unique synergy reaches the optimum at n=3.Besides,as n increases,the proportion of unstable rock-salt layers accordingly decreases and the leaching of ions(especially Sr^(2+))into the electrolyte is suppressed,which induces a decrease in the leaching of active Fe ions,ultimately leading to enhanced stability.This work provides a new avenue for rational catalyst design through the dimensional strategy.

关 键 词：crystal dimensionalities oxygen evolution reaction Ruddlesden-Popper perovskites SYNERGY 

分 类 号：O64[理学—物理化学]