Computational Screening of Bimetallic Catalysts: Application to Ammonia Decomposition,The Journal of Physical Chemistry C

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Computational Screening of Bimetallic Catalysts: Application to Ammonia Decomposition
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-12-21 , DOI: 10.1021/acs.jpcc.1c08091
Hongbo Wu _{1,

2} , Chang Liu ₃ , Wei Guo ₁

Affiliation

First-principles calculations and ab initio molecular dynamics (AIMD) are carried out to perform catalyst screening and investigate the structural dynamics of various transition-metal bimetallic surfaces (guest Fe, Co, and Ni; host Pd, Ag, Ir, Pt, and Au) for ammonia decomposition. First, we identify the activities of stepped/edged bimetallic surfaces using a library of surface N atom (N*) binding energies guided from a scaling-based kinetic Monte Carlo model with a focus on N* coverage effect. Second, based on segregation energy calculations and AIMD simulations, the improved thermodynamic and dynamic stability of bimetallic monolayer and stepped/edged surfaces are illustrated by considering N*–metal interactions. Several active Ir(111)-, Pd(111)-, and Pt(111)-based bimetallic surfaces with well-ordered stripes are found to be stable even without N*. For Ag(111)- and Au(111)-based surfaces, their stability depends on guest atoms’ loading and coverage of N*. In particular, we discover that N* can lead to the spontaneous formation of well-ordered Fe stripes on the Ag(111) surface, a lower N*–N* association barrier (1.74 eV) is observed at step/edge sites, and the striped structure can be preserved in 10 ps’ AIMD simulations at 800 K by N* regulation. Our work offers a family of efficient bimetallic catalysts in ammonia decomposition and provides guidance for tailoring bimetallic surfaces with multifunctionality microstructures in terms of adsorbate-induced catalyst dynamics. This approach also sheds light on other structure-sensitive reactions with complex chemistries to design highly active and stable catalysts under reaction conditions.

中文翻译：

双金属催化剂的计算筛选：在氨分解中的应用

进行第一性原理计算和从头算分子动力学 (AIMD) 以进行催化剂筛选并研究各种过渡金属双金属表面（客体 Fe、Co 和 Ni；主 Pd、Ag、Ir、Pt 和Au) 用于氨分解。首先，我们使用表面 N 原子 (N*) 结合能库识别阶梯/边缘双金属表面的活性，该库由基于缩放的动力学蒙特卡罗模型引导，重点是 N* 覆盖效应。其次，基于偏析能计算和 AIMD 模拟，通过考虑 N*-金属相互作用来说明双金属单层和阶梯/边缘表面的改进的热力学和动态稳定性。几种活性 Ir(111)-、Pd(111)-、发现具有有序条纹的 Pt(111) 基双金属表面即使没有 N* 也是稳定的。对于基于 Ag(111) 和 Au(111) 的表面，它们的稳定性取决于客体原子的负载和 N* 的覆盖。特别是，我们发现 N* 可以导致在 Ag(111) 表面上自发形成有序的 Fe 条纹，在台阶/边缘位置观察到较低的 N*-N* 缔合势垒 (1.74 eV)，并且通过 N* 调节，可以在 800 K 的 10 ps' AIMD 模拟中保留条纹结构。我们的工作为氨分解提供了一系列高效的双金属催化剂，并为在吸附质诱导的催化剂动力学方面定制具有多功能微结构的双金属表面提供了指导。

更新日期：2022-01-13

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