Density functional theory based computational investigations on the stability of highly active trimetallic PtPdCu nanoalloys for electrochemical oxygen reduction
Density functional theory based computational investigations on the stability of highly active trimetallic PtPdCu nanoalloys for electrochemical oxygen reduction
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基于密度泛函理论的高活性三金属 PtPdCu 纳米合金电化学氧还原稳定性的计算研究
DOI：
10.1039/d2fd00101b
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发表时间：
2023
影响因子：
3.4
通讯作者：
Zhong, Chuan-Jian
中科院分区：
文献类型：
--
作者：
Wang, Lichang;Ore, Rotimi M.;Jayamaha, Peshala K.;Wu, Zhi-Peng;Zhong, Chuan-Jian
活性、成本和耐久性是电化学氧还原反应(ORR)的催化研究的三位一体。虽然提高ORR催化剂的活性和降低其成本的研究已经得到了广泛的开展，但高活性ORR催化剂的耐久性研究还需要做大量的工作。在这项工作中，我们用基于密度泛函理论(DFT)的计算考察了三金属PtPdCu催化剂的稳定性，该催化剂在ORR过程中表现出了高活性和令人难以置信的耐久性。具体地说，我们研究了Pt20Pd20Cu60催化剂在高达1.2V的电极电位下，铜物种在表面和内层之间的溶解/沉积和扩散过程，以了解它们对稳定Pt20Pd20Cu60催化剂的作用。结果表明，在富铜PtPdCu纳米合金的晶格常数的稳定性和观察到的振荡中，存在一个由溶解、沉积、从表面向内层扩散和从内层向表面扩散四个过程相互作用的动态铜表面成分范围。
Activity, cost, and durability are the trinity of catalysis research for the electrochemical oxygen reduction reaction (ORR). While studies towards increasing activity and reducing cost of ORR catalysts have been carried out extensively, much effort is needed in durability investigation of highly active ORR catalysts. In this work, we examined the stability of a trimetallic PtPdCu catalyst that has demonstrated high activity and incredible durability during ORR using density functional theory (DFT) based computations. Specifically, we studied the processes of dissolution/deposition and diffusion between the surface and inner layer of Cu species of Pt20Pd20Cu60 catalysts at electrode potentials up to 1.2 V to understand their role towards stabilizing Pt20Pd20Cu60 catalysts. The results show there is a dynamic Cu surface composition range that is dictated by the interplay of the four processes, dissolution, deposition, diffusion from the surface to inner layer, and diffusion from the inner layer to the surface of Cu species, in the stability and observed oscillation of lattice constants of Cu-rich PtPdCu nanoalloys.