Deciphering Water Oxidation Catalysts:The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity PromotionOA
Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity enhancement.Here,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is reported.The substituting Fe content influences both current change tendency and surface reconstruction degree.LaNi_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)series.The reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based catalysts.Besides,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability.Furthermore,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree.The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction.This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.
Li An;Jianyi Li;Yuanmiao Sun;Jiamin Zhu;Justin Zhu Yeow Seow;Hong Zhang;Nan Zhang;Pinxian Xi;Zhichuan J.Xu;Chun‑Hua Yan
State Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou 730000,People’s Republic of ChinaState Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou 730000,People’s Republic of ChinaSchool of Materials Science and Engineering,Nanyang Technological University,Singapore 639798,Singapore Faculty of Materials Science and Energy Engineering,Institute of Technology for Carbon Neutrality,Shenzhen Institute of Advanced Technology,Chinese Academy of Sciences,Shenzhen 518055,People’s Republic of ChinaState Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou 730000,People’s Republic of ChinaSchool of Materials Science and Engineering,Nanyang Technological University,Singapore 639798,SingaporeKey Laboratory of Electromagnetic Materials and Devices,National Center for International Research On Photoelectric and Energy Materials,School of Materials and Energy,Electron Microscopy Center,Yunnan University,Kunming 650091,People’s Republic of ChinaState Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou 730000,People’s Republic of ChinaState Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou 730000,People’s Republic of China State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization,Baotou Research Institute of Rare Earths,Baotou 014030,People’s Republic of ChinaSchool of Materials Science and Engineering,Nanyang Technological University,Singapore 639798,SingaporeState Key Laboratory of Applied Organic Chemistry,Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province,Frontiers Science Center for Rare Isotopes,College of Chemistry and Chemical Engineering,Lanzhou University,Lanzhou 730000,People’s Republic of China Beijing National Laboratory for Molecular Sciences,State Key Laboratory of Rare Earth Materials Chemistry and Applications,PKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry,Peking University,Beijing 100871,People’s Republic of China
化学
Oxygen evolution reactionPerovskite oxidesDopingActivation and reconstruction
《Nano-Micro Letters》 2025 (3)
P.340-354,15
funded by the National Key R&D Program of China(2021YFA1501101)the National Natural Science Foundation of China(No.22471103,22425105,22201111,21931001,22221001,and 22271124)Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province(2019ZX-04)the 111 Project(B20027)as well as the National Natural Science Foundation of Gansu Province(22JR5RA470)the Fundamental Research Funds for the Central Universities(lzujbky-2023-eyt03)supported by the Agency for Science,Technology and Research(A*STAR)MTC Individual Research Grants(IRG)M22K2c0078.
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