Experimental Sabatier plot for predictive design of active and stable Pt-alloy oxygen reduction reaction catalysts
Experimental Sabatier plot for predictive design of active and stable Pt-alloy oxygen reduction reaction catalysts
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DOI：
10.1038/s41929-022-00797-0
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发表时间：
2022-06-09
期刊：
影响因子：
37.8
通讯作者：
Huang, Yu
中科院分区：
文献类型：
--
作者：
Huang, Jin;Sementa, Luca;Huang, Yu
质子交换膜燃料电池广泛采用的一个关键技术障碍是开发高活性和耐用的铂基催化剂，用于加速缓慢的氧还原反应，迄今为止，这在很大程度上依赖于轶事发现。虽然氧结合能Δ E-O经常被用作预测活性的理论描述符，但没有已知的用于预测耐久性的描述符。在这里，我们开发了一个二进制的实验描述符，捕获应变和Pt过渡金属耦合的贡献，通过X-射线吸收光谱和直接相关的二进制实验描述符与计算的Δ E-O的催化剂表面。这导致了实验验证的Sabatier图来预测宽范围的Pt合金氧还原反应催化剂的催化活性和稳定性。在此基础上，进一步设计了一种同时具有高活性和高稳定性的氧还原反应催化剂。
A critical technological roadblock to the widespread adoption of proton-exchange membrane fuel cells is the development of highly active and durable platinum-based catalysts for accelerating the sluggish oxygen reduction reaction, which has largely relied on anecdotal discoveries so far. While the oxygen binding energy Delta E-O has been frequently used as a theoretical descriptor for predicting the activity, there is no known descriptor for predicting durability. Here we developed a binary experimental descriptor that captures both the strain and Pt transition metal coupling contributions through X-ray absorption spectroscopy and directly correlated the binary experimental descriptor with the calculated Delta E-O of the catalyst surface. This leads to an experimentally validated Sabatier plot to predict both the catalytic activity and stability for a wide range of Pt-alloy oxygen reduction reaction catalysts. Based on the binary experimental descriptor, we further designed an oxygen reduction reaction catalyst wherein high activity and stability are simultaneously achieved.