脱质子化
化学
离解(化学)
化学物理
析氧
质子
氧气
价(化学)
溶解
缩放比例
接受者
价键理论
工作(物理)
计算化学
质子输运
键裂
氧气输送
电解质
电催化剂
光化学
质子交换膜燃料电池
反应机理
物理化学
线性比例尺
反应中间体
膜
分解水
过渡状态
作者
Jixiang Jiao,Hongyu Zhao,Ying Dong,Ding Chen,Linbo Jiang,Xu Luo,Bingqing Tian,Guozhuang Li,Junxin Duan,Shichun Mu
摘要
ABSTRACT Oxygen evolution reaction electrocatalysts following the adsorbate evolution mechanism (AEM) exhibit exceptional structural stability, but the activity is inherently constrained by the linear scaling relationship associated with single‐metal sites. Here, we propose a metal‐site proton‐acceptor‐assisted deprotonation AEM (MP‐AEM) by incorporating Pd into RuO 2 as secondary metal‐site proton acceptors to activate a novel proton‐transfer pathway. Theoretical calculations and operando characterizations confirm that Pd‐RuO 2 generates new intermediates, reducing the rate‐determining energy barrier by 0.41 eV. Moreover, Pd proton acceptor lowers the O─H bond dissociation barrier and optimizes the hydrogen‐bond network, thereby accelerating the deprotonation kinetics. Furthermore, reduced Ru valence and weakened Ru─O covalency inhibit Ru oxidative dissolution and the lattice‐oxygen‐mediated mechanism. The Pd‐RuO 2 applied in proton exchange membrane water electrolyzers (PEMWEs) requires only 1.55 V @ 1 A cm −2 and shows 15‐fold higher stability than pure RuO 2 . This work establishes an innovative pathway and insight for designing highly efficient PEMWEs catalysts.
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