Design and screening of bimetallic catalysts for nitric oxide reduction by CO: a study of kinetic Monte Carlo simulation based on first-principles calculations,Physical Chemistry Chemical Physics

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Design and screening of bimetallic catalysts for nitric oxide reduction by CO: a study of kinetic Monte Carlo simulation based on first-principles calculations
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2024-09-04 , DOI: 10.1039/d4cp02613f
Caimu Wang ₁ , Renyi Li ₁ , Wei Guo _{1,

2}

Affiliation

Nitric oxide (NO) emissions pose a significant environmental challenge, and the development of effective catalysts for NO reduction is crucial. This study investigates the potential of striped bimetallic catalysts for NO reduction by CO using kinetic Monte Carlo (KMC) simulations based on first-principles calculations. The simulations reveal that the activity on the striped Ni–Pt–Pt (111) surface is 1–2 orders of magnitude higher than that on the terraced Ni–Pt–Pt (111) surface at the same temperatures, demonstrating the importance of defect engineering. Sensitivity analysis identifies CO oxidation as the rate-determining step, although the 2N* association barrier is higher than CO oxidation, highlighting the need to consider reaction conditions in kinetic simulations. Volcano plots based on the formation energies of NO* and CO* successfully predict the striped Ni–Pd–Pd (111) and Ni–Rh–Rh (111) surfaces as optimal catalysts, which were further validated through DFT calculations and ab initio molecular dynamics simulations. This study offers valuable insights for designing high-performance bimetallic catalysts for NO reduction and underscores the importance of considering specific reaction conditions in kinetic simulations.

中文翻译：

CO还原一氧化氮双金属催化剂的设计与筛选：基于第一性原理计算的动力学蒙特卡罗模拟研究

一氧化氮 (NO) 排放对环境造成了重大挑战，开发有效的 NO 还原催化剂至关重要。本研究利用基于第一性原理计算的动力学蒙特卡罗 (KMC) 模拟，研究了条纹双金属催化剂通过 CO 还原 NO 的潜力。模拟结果表明，在相同温度下，条状 Ni-Pt-Pt (111) 表面的活性比阶梯状 Ni-Pt-Pt (111) 表面的活性高 1-2 个数量级，这证明了缺陷的重要性工程。灵敏度分析将 CO 氧化确定为速率决定步骤，尽管 2N* 缔合势垒高于 CO 氧化，这强调了在动力学模拟中需要考虑反应条件。基于 NO* 和 CO* 形成能的火山图成功预测了条纹 Ni-Pd-Pd (111) 和 Ni-Rh-Rh (111) 表面作为最佳催化剂，并通过 DFT 计算和从头算分子进一步验证动力学模拟。这项研究为设计用于还原 NO 的高性能双金属催化剂提供了宝贵的见解，并强调了在动力学模拟中考虑特定反应条件的重要性。

更新日期：2024-09-04

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