The development of anodic electrocatalysts toward the oxygen evolution reaction(OER)in harsh acidic environments faces significant challenges of low efficiency,instability and high cost.Ru-based oxides exhibit remarka...The development of anodic electrocatalysts toward the oxygen evolution reaction(OER)in harsh acidic environments faces significant challenges of low efficiency,instability and high cost.Ru-based oxides exhibit remarkable initial activity toward the OER,but the presence of soluble high-valence oxygenvacancy intermediates can accelerate the dissolution of Ru species.In this study,a triple Sr2CaRu2IrO9 perovskite oxide electrocatalyst has been successfully synthesized,demonstrating a low overpotential of 172 mV at 10 mA cm^(-2)and excellent stability for over 75 hours.The introduction of dual-site heteroatoms leads to the generation of oxygen vacancies,which control the excessive lattice oxygen participating in the OER via the lattice oxygen oxidation mechanism(LOM).This effectively prevents the excessive oxidation of Ru to form soluble Ru^(>4+)species.Density functional theory(DFT)calculations show that the negative shift of O 2p and Ru 4d band centers weakens the covalency of Ru-O,optimizes the adsorption energy of oxygen intermediates,and thus improves the inherent catalytic activity and stability.展开更多
基金the financial support from the National Natural Science Foundation of China(NSFC,grant no.52073283,22078124,and 22378158)Natural Science Foundation Project of Jilin Province(YDZJ202201ZYTS336)+4 种基金Key Projects of Science and Technology Development Plan of Jilin Province(20220201125GX)the Project of Education Department of Jilin Province(JJKH20221155KJ)the Project of Jilin Province Development and Reform Commission(2023C032-2 and 2023C032-5)the Program for the Development of Science and Technology of Jilin Province(20230508040RC)the Science and Technology Innovation Center Project of Jilin Province(YDZJ202102CXJD049).
文摘The development of anodic electrocatalysts toward the oxygen evolution reaction(OER)in harsh acidic environments faces significant challenges of low efficiency,instability and high cost.Ru-based oxides exhibit remarkable initial activity toward the OER,but the presence of soluble high-valence oxygenvacancy intermediates can accelerate the dissolution of Ru species.In this study,a triple Sr2CaRu2IrO9 perovskite oxide electrocatalyst has been successfully synthesized,demonstrating a low overpotential of 172 mV at 10 mA cm^(-2)and excellent stability for over 75 hours.The introduction of dual-site heteroatoms leads to the generation of oxygen vacancies,which control the excessive lattice oxygen participating in the OER via the lattice oxygen oxidation mechanism(LOM).This effectively prevents the excessive oxidation of Ru to form soluble Ru^(>4+)species.Density functional theory(DFT)calculations show that the negative shift of O 2p and Ru 4d band centers weakens the covalency of Ru-O,optimizes the adsorption energy of oxygen intermediates,and thus improves the inherent catalytic activity and stability.
