Role of A-sites in pyrochlore lanthanide ruthenate for electrocatalysis of oxygen evolution reaction  

作　　者：Hengyu Guo Zhengping Zhang Feng Wang 

机构地区：[1]State Key Laboratory of Chemical Resource Engineering,Beijing Key Laboratory of Electrochemical Process and Technology for Materials,Beijing University of Chemical Technology,Beijing,100029,China [2]Beijing Advanced Innovation Center for Soft Matter Science and Engineering,Beijing University of Chemical Technology,Beijing,100029,China

出　　处：《Journal of Materiomics》2024年第6期1234-1242,共9页无机材料学学报（英文）

基　　金：This work was supported by the National Key R&D Program of China[2022YFE0110400];the National Natural Science Foundation of China[52122207,52173245,U20A20337,52130206,and 52221006];the Fundamental Research Funds for the Central Universities[CLYY2022].

摘　　要：Developing highly stable and efficient catalysts for oxygen evolution reaction(OER)is extremely important to sustainable energy conversion and storage,but improved efficiency is largely hindered by sluggish reaction kinetics.Dense and bimetal ruthenates have emerged as one of the promising substitutes to replace single-metal ruthenium or iridium oxides,but the fundamental understanding the role of A-site cations is still blurring.Herein,a family of lanthanides(Ln=all the lanthanides except Pm)are applied to synthesize pyrochlore lanthanide ruthenates(Ln_(2)Ru_(2)O_(7)),and only Ln_(2)Ru_(2)O_(7)(Ln=Sm,Eu,Gd,Tb,Dy,Ho,Er,Tm,Yb,or Lu)with pure phase can be obtained by the ambient-pressure calcination.Compared with the perovskite ruthenates(SrRuO_(3))and rutile RuO_(2),the[RuO_(6)]units in these Ln_(2)Ru_(2)O_(7) present the largely distorted configurations and different energy level splitting to prevent the excessive Ru oxidation and dissolution,which leads the primary improvement in the electrocatalytic OER performance.In the similar crystalline field split states,the charge transfer between[RuO_(6)]units and Ln^(3+)cations also affect catalytic activities,even in the Ln_(2)Ru_(2)O_(7) surface reconstruction during the OER process.Consequently,Tb_(2)Ru_(2)O_(7) showed the highest OER performance among all the prepared Ln_(2)Ru_(2)O_(7) with similar morphologies and crystallization.This systematic work gives fundamental cognition to rational design of high-performance OER electrocatalysts in proper water electrolysis technologies.

关 键 词：PYROCHLORES LANTHANIDES RUTHENATES Electrocatalysts Oxygen evolution reaction 

分 类 号：O64[理学—物理化学]