Department of Chemistry and Biochemistry, Graduate School of Humanities and Sciences, Ochanomizu University, 2-1-1 Otsuka, Bunkyo-ku, Tokyo 112-8610, Japan.
Faculty of Core Research Natural Science Division, Ochanomizu University, 2-1-1 Otsuka, Bunkyo-ku, Tokyo 112-8610, Japan.
Sci Rep. 2017 Mar 28;7:45381. doi: 10.1038/srep45381.
In the present study, methods to enhance the oxygen reduction reaction (ORR) activity of sub-nanosized Pt clusters were investigated in a theoretical manner. Using ab initio molecular dynamics and Monte Carlo simulations based on density functional theory, we have succeeded in determining the origin of the superior ORR activity of Pt compared to that of Pt. That is, it was clarified that the electronic structure of Pt fluctuates to a greater extent compared to that of Pt, which leads to stronger resistance against catalyst poisoning by O/OH. Based on this conclusion, a set of sub-nanosized Pt-alloy clusters was also explored to find catalysts with better ORR activities and lower financial costs. It was suggested that GaPt, GePt, and SnPt would be good candidates for ORR catalysts.
在本研究中，我们以理论方式研究了增强亚纳 米级 Pt 团簇氧还原反应（ORR）活性的方法。通过基于密度泛函理论的从头算分子动力学和蒙特卡罗模拟，我们成功确定了 Pt 相较于 Pt 具有更高 ORR 活性的原因。也就是说，阐明了 Pt 的电子结构比 Pt 的电子结构波动更大，这导致其对 O/OH 的催化剂中毒具有更强的抵抗力。基于这一结论，我们还探索了一组亚纳 米级 Pt 合金团簇，以寻找具有更好 ORR 活性和更低经济成本的催化剂。研究表明，GaPt、GePt 和 SnPt 将是良好的 ORR 催化剂候选物。
