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Improving the Hydrogen Oxidation Reaction Rate of Ru by Active Hydrogen in the Ultrathin Pd Interlayer
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-02 , DOI: 10.1021/jacs.3c02604 Xianmeng Song 1 , Xia-Guang Zhang 2 , Yong-Liang Deng 1 , Zi-Ang Nan 1 , Weishen Song 1 , Yanjie Wang 1 , Linzhe Lü 1 , Qiaorong Jiang 1 , Xi Jin 1 , Yanping Zheng 1 , Mingshu Chen 1 , Zhaoxiong Xie 1 , Jian-Feng Li 1, 3 , Zhong-Qun Tian 1 , Feng Ru Fan 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-02 , DOI: 10.1021/jacs.3c02604 Xianmeng Song 1 , Xia-Guang Zhang 2 , Yong-Liang Deng 1 , Zi-Ang Nan 1 , Weishen Song 1 , Yanjie Wang 1 , Linzhe Lü 1 , Qiaorong Jiang 1 , Xi Jin 1 , Yanping Zheng 1 , Mingshu Chen 1 , Zhaoxiong Xie 1 , Jian-Feng Li 1, 3 , Zhong-Qun Tian 1 , Feng Ru Fan 1
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Enhancing the catalytic activity of Ru metal in the hydrogen oxidation reaction (HOR) potential range, improving the insufficient activity of Ru caused by its oxophilicity, is of great significance for reducing the cost of anion exchange membrane fuel cells (AEMFCs). Here, we use Ru grown on Au@Pd as a model system to understand the underlying mechanism for activity improvement by combining direct in situ surface-enhanced Raman spectroscopy (SERS) evidence of the catalytic reaction intermediate (OHad) with in situ X-ray diffraction (XRD), electrochemical characterization, as well as DFT calculations. The results showed that the Au@Pd@Ru nanocatalyst utilizes the hydrogen storage capacity of the Pd interlayer to “temporarily” store the activated hydrogen enriched at the interface, which spontaneously overflows at the “hydrogen-deficient interface” to react with OHad adsorbed on Ru. It is the essential reason for the enhanced catalytic activity of Ru at anodic potential. This work deepens our understanding of the HOR mechanism and provides new ideas for the rational design of advanced electrocatalysts.
中文翻译：
超薄Pd夹层活性氢提高Ru的氢氧化反应速率
提高Ru金属在氢氧化反应（HOR）电位范围内的催化活性，改善Ru因其亲氧性而导致的活性不足，对于降低阴离子交换膜燃料电池（AEMFCs）的成本具有重要意义。在这里，我们使用在 Au@Pd 上生长的 Ru 作为模型系统，通过结合催化反应中间体（OH ad) 与原位 X 射线衍射 (XRD)、电化学表征以及 DFT 计算。结果表明，Au@Pd@Ru纳米催化剂利用Pd夹层的储氢能力，“暂时”储存界面富集的活性氢，在“缺氢界面”自发溢出与吸附的OH发生反应在茹。这是提高 Ru 在阳极电位下催化活性的根本原因。这项工作加深了我们对HOR机制的理解，为先进电催化剂的合理设计提供了新思路。
更新日期：2023-06-02
中文翻译：
超薄Pd夹层活性氢提高Ru的氢氧化反应速率
提高Ru金属在氢氧化反应（HOR）电位范围内的催化活性，改善Ru因其亲氧性而导致的活性不足，对于降低阴离子交换膜燃料电池（AEMFCs）的成本具有重要意义。在这里，我们使用在 Au@Pd 上生长的 Ru 作为模型系统，通过结合催化反应中间体（OH ad) 与原位 X 射线衍射 (XRD)、电化学表征以及 DFT 计算。结果表明，Au@Pd@Ru纳米催化剂利用Pd夹层的储氢能力，“暂时”储存界面富集的活性氢，在“缺氢界面”自发溢出与吸附的OH发生反应在茹。这是提高 Ru 在阳极电位下催化活性的根本原因。这项工作加深了我们对HOR机制的理解，为先进电催化剂的合理设计提供了新思路。
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