High-entropy perovskite oxides: A versatile class of materials for nitrogen reduction reactions

作     者：Kaibin Chu Jingjing Qin Haiyan Zhu Michiel De Ras Chuang Wang Lei Xiong Longsheng Zhang Nan Zhang Johan A.Martens Johan Hofkens Feili Lai Tianxi Liu 楚凯斌;秦静静;朱海燕;Michiel De Ras;王闯;熊磊;张龙生;张楠;Johan A.Martens;Johan Hofkens;赖飞立;刘天西

作者机构：The Key Laboratory of Synthetic and Biological ColloidsMinistry of EducationSchool of Chemical and Material EngineeringInternational Joint Research Laboratory for Nano Energy CompositesJiangnan UniversityWuxi 214122China Department of ChemistryKU LeuvenCelestijnenlaan 200FLeuven 3001Belgium State Key Laboratory of Food Science and TechnologyJiangnan UniversityWuxi 214122China Centre of Surface Chemistry and Catalysis:Characterisation and Application TeamKU LeuvenLeuven 3001Belgium Max Planck Institute for Polymer ResearchAckermannweg 10Mainz 55128Germany 

出 版 物：《Science China Materials》 (中国科学（材料科学（英文版）)

年 卷 期：2022年第65卷第10期

页      面：2711-2720页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：supported by the National Natural Science Foundation of China (52161135302, 21674019, and 51801075) the Research Foundation Flanders (G0F2322N) Shanghai Scientific and Technological Innovation Project (18JC1410600) the Program of the Shanghai Academic Research Leader (17XD1400100) the financial support from the Flemish Government through the Moonshot cSBO project P2C (HBC.2019.0108) the Long-term Structural Funding (Methusalem CASAS2, Meth/15/04) Interne Fondsen KU Leuven through project C3/20/067 the support from the Research Foundation-Flanders (FWO) in the form of a doctoral fellowship (1SA3321N) the financial support from China Scholarship Council in the form of a visiting Ph.D. Student (File No. 202106790090) the LvLiang Cloud Computing Center of China, and the calculations were performed on a TianHe-2 system the characterizations supported by the Central Laboratory, School of Chemical and Material Engineering, Jiangnan University 

主　　题：high entropy perovskite nitrogen reduction reaction catalytic activity center 

摘      要：Despite the intense research efforts directed to electrocatalytic nitrogen reduction reaction(eNRR),the NH_(3) yield and selectivity are still not up to the standard of practical ***,high-entropy perovskite oxides with composition Bax(FeCoNiZrY)_(0.2)O_(3−δ)(Bx(FCNZY)_(0.2)(x=0.9,1)are reported as eNRR *** eNRR activity of high-entropy perovskite oxide is enhanced by changing the nonstoichiometric metal elements at the A-site,thus generating additional oxygen *** NH_(3) yield and Faraday efficiency for B_(0.9)(FCNZY)_(0.2) are 1.51 and 1.95 times higher than those for B(FCNZY)_(0.2),*** d-band center theory is used to theoretically predict the catalytically active center at the B-site,and as a result,nickel was identified as the catalytic *** free energy values of the intermediate states in the optimal distal pathway show that the third protonation step(*NNH_(2)→*NNH_(3))is the rate-determining step and that the increase in oxygen vacancies in the high-entropy perovskite contributes to nitrogen adsorption and *** work provides a framework for applying high-entropy structures with active site diversity for electrocatalytic nitrogen fixation.