分解水
密度泛函理论
化学
析氧
催化作用
纳米材料基催化剂
氢
电子转移
化学物理
工作职能
光化学
计算化学
物理化学
光催化
生物化学
有机化学
电极
电化学
作者
Yiqiang Sun,Chenchen Wang,Yong Wang,Yujuan Xu,Xiaodong Yang,Bo Ouyang,Cuncheng Li
标识
DOI:10.1016/j.apsusc.2023.159222
摘要
Water splitting, one of the primary strategies for advancing the utilization of hydrogen production, necessitates the input of external energies to initiate the reaction due to its thermodynamically uphill nature. Nevertheless, Ru-based compounds, which were widely used as benchmark anodic catalysts, facing significant drawbacks such as their susceptibility to dissolution, significantly restrict the overall water splitting efficiency. In this work, we introduce an approach for functionalization through combining Ru nanospheres with Ir to form a Ru@Ir core–shell structure (denoted as Ru@Ir core–shell NSs), which can activate the superior oxygen evolution reaction (OER) catalytic activity, and simultaneously inherit the hydrogen evolution reaction (HER) performance in all-pH condition. The work function difference between Ru and Ir promotes the necessary energetic impetus for electron migration from Ru to Ir, resulting in the charge redistribution. Density functional theory (DFT) calculations confirmed that the Ir shell, acting as an electron acceptor, could effectively trigger electron rearrangement, augmenting the ligand affinity of hydrogen and oxygen intermediates to attain the most favorable energy states, thereby accelerating the kinetics of hydrogen and oxygen evolution. Our suggested core–shell structure approach for manipulating interface charge distribution might find utility in creating other electrocatalysts for water splitting.
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