化学
电催化剂
插层(化学)
三氧化钨
氧化物
钨
无机化学
催化作用
氢
密度泛函理论
金属
分解水
石墨烯
反应性(心理学)
钨化合物
电化学
纳米技术
物理化学
计算化学
材料科学
有机化学
替代医学
病理
医学
光催化
电极
作者
Evan V. Miu,James R. McKone,Giannis Mpourmpakis
摘要
Metal oxides are attracting increased attention as electrocatalysts owing to their affordability, tunability, and reactivity. However, these materials can undergo significant chemical changes under reaction conditions, presenting challenges for characterization and optimization. Herein, we combine experimental and computational methods to demonstrate that bulk hydrogen intercalation governs the activity of tungsten trioxide (WO3) toward the hydrogen evolution reaction (HER). In contrast to the focus on surface processes in heterogeneous catalysis, we demonstrate that bulk oxide modification is responsible for experimental HER activity. Density functional theory (DFT) calculations reveal that intercalation enables the HER by altering the acid-base character of surface sites and preventing site blocking by hydration. First-principles microkinetic modeling supports that the experimental HER rates can only be explained by intercalated HxWO3, whereas nonintercalated WO3 does not catalyze the HER. Overall, this work underscores the critical influence of hydrogen intercalation on aqueous cathodic electrocatalysis at metal oxides.
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