Bond engineering:weakening Ru-O covalency for efficient and stable water oxidation in acidic solutions  

作　　者：Yifan Yang Jingtong Guo Lixiong Xu Chenyue Li Rongqian Ning Jun Ma Shuo Geng 

机构地区：[1]Guizhou Provincial Key Laboratory of Green Chemical and Clean Energy Technology,School of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,Guizhou,China

出　　处：《Journal of Energy Chemistry》2025年第3期1-9,共9页能源化学(英文版)

基　　金：supported by Young Project of Education Department in Guizhou Province(No.2022099);the Natural Science Special of Guizhou University(No.X202220 Special Post A);the National Natural Science Foundation of China(Grant No.22208071)。

摘　　要：The persistent stability of ruthenium dioxide(RuO_(2))in acidic oxygen evolution reactions(OER)is compromised by the involvement of lattice oxygen(LO)and metal dissolution during the OER process.Heteroatom doping has been recognized as a viable strategy to foster the stability of RuO_(2)for acidic OER applications.This study presented an ion that does not readily gain or lose electrons,Ba^(2+),into RuO_(2)(Ba-RuO_(2))nanosheet(NS)catalyst that increased the number of exposed active sites,achieving a current density of 10 mA/cm^(2)with an overpotential of only 229 mV and sustaining this output for over 250 h.According to density functional theory(DFT)and X-ray absorption spectroscopy,Ba doping resulted in a longer Ru-O bond length,which in turn diminished the covalency of the bond.This alteration curtailed the involvement of LO and the dissolution of ruthenium(Ru),thereby markedly improving the durability of the catalyst over extended periods.Additionally,attenuated total reflectance-surface enhanced infrared absorption spectroscopy analysis substantiated that the OER mechanism shifted from a LO-mediated pathway to an adsorbate evolution pathway due to Ba doping,thereby circumventing Ru over-oxidation and further enhancing the stability of RuO_(2).Furthermore,DFT findings uncovered that Ba doping optimizes the adsorption energy of intermediates,thus enhancing the OER activity in acidic environments.This study offers a potent strategy to guide future developments on Ru-based oxide catalysts'stability in an acidic environment.

关 键 词：Oxygen evolution reaction in acid Bond covalency Rutheniumoxide Ba doping 

分 类 号：O643.36[理学—物理化学]