Computational high-throughput screening of alloy nanoclusters for electrocatalytic hydrogen evolution
Computational high-throughput screening of alloy nanoclusters for electrocatalytic hydrogen evolution
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DOI：
10.1038/s41524-021-00514-8
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发表时间：
2021-04
影响因子：
9.7
通讯作者：
Xinnan Mao;Lu Wang;Yafeng Xu;Pengju Wang;Youyong Li;Jijun Zhao
中科院分区：
文献类型：
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作者：
Xinnan Mao;Lu Wang;Yafeng Xu;Pengju Wang;Youyong Li;Jijun Zhao
在这里，我们报告了一个基于密度泛函理论（DFT）的高通量筛选方法，成功地确定了一种类型的合金纳米团簇作为析氢反应（HER）的电催化剂。对7924个Cu基合金团簇Cu 55-nMn（M = Co，Ni，Ru，Rh）进行了优化和评价，筛选出了有希望的催化剂。通过比较不同的结构模式，Cu基合金团簇更倾向于以掺杂金属为核，Cu为壳原子的核-壳结构。一般来说，过渡金属的掺杂可以显著提高Cu基纳米团簇的HER性能，其活性位主要是外层Cu原子上的桥位和三重位。综合考虑结构稳定性和电化学活性，认为核壳结构的CuNi合金团簇是性能较好的上级析氢电催化剂。提出了一个描述符组成的表面电荷有效地评估支持的DFT计算和机器学习技术的合金团簇的HER活性。我们的筛选策略可以加快发现有前途的HER电催化剂使用金属合金纳米团簇的步伐。
Here, we report a density functional theory (DFT)-based high-throughput screening method to successfully identify a type of alloy nanoclusters as the electrocatalyst for hydrogen evolution reaction (HER). Totally 7924 candidates of Cu-based alloy clusters of Cu55-nMn(M = Co, Ni, Ru, and Rh) are optimized and evaluated to screening for the promising catalysts. By comparing different structural patterns, Cu-based alloy clusters prefer the core–shell structures with the dopant metal in the core and Cu as the shell atoms. Generally speaking, the HER performance of the Cu-based nanoclusters can be significantly improved by doping transition metals, and the active sites are the bridge sites and three-fold sites on the outer-shell Cu atoms. Considering the structural stability and the electrochemical activity, core–shell CuNi alloy clusters are suggested to be the superior electrocatalyst for hydrogen evolution. A descriptor composing of surface charge is proposed to efficiently evaluate the HER activity of the alloy clusters supported by the DFT calculations and machine-learning techniques. Our screening strategy could accelerate the pace of discovery for promising HER electrocatalysts using metal alloy nanoclusters.