Yueying Yan , Tian Meng , Yuting Chen , Yang Yang , Dewen Wang , Zhicai Xing , Xiurong Yang
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引用次数: 0
Abstract
The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction (HER). Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of HER. In this study, RuO2/BaRuO3 (RBRO) heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of gel-precursor. The RBRO heterostructures obtained at 550 °C exhibited the highest HER activity in 1 M KOH, showing an ultra-low overpotential of 16 mV at 10 mA cm−2 and a Tafel slope of 33.37 mV dec−1. Additionally, the material demonstrated remarkable durability, with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm−2. Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H* and OH* and effectively lower the energy barrier of water dissociation. This research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.
在碱性析氢反应(HER)中,水缓慢解离是减慢反应速率的决定速率步骤。优化催化剂的表面电子结构,降低水解离能垒,调节吸附中间体的结合强度是提高HER催化性能的关键策略。本研究通过凝胶前驱体的热分解,在低温下原位构建了具有丰富氧空位和晶格畸变的RuO2/BaRuO3 (RBRO)异质结构。在550°C下得到的RBRO异质结构在1 M KOH下表现出最高的HER活性,在10 mA cm−2下表现出16 mV的超低过电位,Tafel斜率为33.37 mV dec−1。此外,该材料表现出了显著的耐久性,在10 mA cm - 2下进行200小时的稳定性测试后,过电位仅下降了25 mV。密度泛函理论计算表明,电荷在异质结界面的重新分配可以优化H*和OH*的结合能,有效降低水解离的能垒。本研究通过系统设计非均相界面,为突破碱性HER催化剂的水解离阈值提供了新的视角。