化学工程2026，Vol.54Issue(6)：29-34,6.DOI:10.3969/j.issn.1005-9954.2026.06.005
基于分子模拟的Pt/Cu基催化剂NH3-SCO反应性能
Performance of Pt/Cu based catalyst for NH3-SCO reaction based on molecular simulation
摘要
Abstract
Molecular dynamics and first-principles simulations were employed based on the Materials Studio software to systematically investigate the reaction mechanisms of Pt/Al2O3,Pt/TiO2 and Cu/Al2O3 catalysts in ammonia oxidation.Experimental validation was used to analyze the regulatory effects of support properties and active components on catalytic performance.The molecular dynamics simulations,performed using the Sorption and Forcite modules,revealed the adsorption and diffusion behaviors of gas molecules on the surfaces of the three catalyst types.Al2O3 support exhibits a significantly higher absolute adsorption capacity for NH3 within 100-400 ℃compared to TiO2 support.NH3 demonstrates the highest diffusion coefficient of 3.5 × 10-8 m2/s on Cu/Al2O3 surface at 400℃.First-principles calculations,conducted using the Dmol3 module,comparatively analyzed the reaction pathway differences between Pt-based and Cu-based catalysts.Ammonia oxidation on Pt-based catalyst surfaces follows a stepwise dehydrogenation pathway,with N—N bond formation presenting a high energy barrier of 1.347 eV,acting as the rate-determining step.In contrast,Cu/Al2O3 directly generates N2 via—NH3 coupling pathway(—NH3→ N2H4→ N2),where the key energy barrier is clearly lower than that in Pt-based systems.This study reveals the synergistic regulation of support acidic sites and metal-support interactions on the selectivity of reaction pathways:Al2O3 enhances reactant enrichment efficiency through strong chemisorption,and TiO2 relies on physical adsorption to promote intermediate desorption.关键词
NH3-SCO催化剂/分子动力学/第一性原理/NH3吸附扩散/反应路径Key words
NH3-SCO catalyst/molecular dynamics/first-principles/NH3 adsorption and diffusion/reaction pathway分类
能源科技引用本文复制引用
张光辉,陈昊,聂学选,张鹏,陈占明,王小琛..基于分子模拟的Pt/Cu基催化剂NH3-SCO反应性能[J].化学工程,2026,54(6):29-34,6.基金项目
国家自然科学基金资助项目(22272010) （22272010）
陕西省创新能力支撑计划项目(2021TD-28) （2021TD-28）
