用量子理论对煤粉再燃中NH自由基与NO反应的物化研究  

Study on NH and NO Physical and Chemical Reaction in Coal Powder Reburning by Quantum Theory

作　　者：吴高贺[1] 杜梅芳[1] 侯宁普[1] 张影[1] 鲁贵林[1] 张忠孝[1] 

机构地区：[1]上海理工大学理学院,上海200093

出　　处：《材料导报》2011年第14期144-146,共3页Materials Reports

基　　金：国家自然科学基金项目(50906055)

摘　　要：对气体再燃低NOx燃烧过程进行分析,采用量子化学密度泛函理论研究了NH自由基与NO反应的机理,优化了反应过程中反应物、中间体、过渡态和产物的几何构型,并计算了它们的能量,同时对它们进行振动分析,以确定中间体和过渡态的真实性。对NH自由基与NO反应机理进行了比较,并通过模拟NH自由基与NO的反应,得出通道NO+NH→IM3→TS1→IM4→N2+OH的活化能(100.03kJ/mol)最低,为主要反应通道。揭示其微观机理,对认识再燃脱硝的本质和主要过程具有重要的理论参考价值和实践指导意义。This research mainly focuses on the low-NOx combustion analysis of gas reburning process, the study of NH radical with NO reaction mechanism using the quantum chemical density functional theory and the products geometry of reactants,intermediates,transition states during the optimizing reaction process. Their energy was calculated, and meanwhile, their vibration analysis was carried out to determine the intermediates and transition states. Verified the NH radical and NO reaction mechanism, the channel NO ＋ NH→IM3-2 TS1 →IM4→N2＋OH with activation energy（100.03kJ/mol） minimum was obtained, as the main reaction channel. Revealing the microscopic mechanism has important theoretical reference and practical guide on the understanding of the nature of reburning NO, and prima ry process.

关 键 词：NH自由基 反应机理 过渡态 反应通道 活化能 

分 类 号：O641[理学—物理化学]