N2O在氧化镍表面催化的机理研究吴洋文.docxVIP

摘要N2O是一种对大气环境有很大破坏作用的温室气体，吸收红外辐射、引起全球变暖的能力极强。近年来，随着人们环保意识的不断增强，N2O的脱除技术受到了越来越多环境保护领域研究人员的关注。其中直接催化分解法由于反应温度低、不需还原剂、运行费用低，且分解所得产物N2和O2对环境没有二次污染等优点，已成为目前最有应用前景的N2O脱除技术。研究表明，NiO作为一种金属氧化物催化剂其分解N2O的效率较高。基于量子化学理论，通过密度泛函理论（DFT)和Materials Studio软件的CASTEP模块构建了NiO(100)表面，并利用其DMol3模块，结构优化采用广义梯度近似(GGA)，密度泛函选取PBE形式，探讨了在NiO(100)表面N2O分解的机理。通过DMol3模块的TS search功能搜索过渡态，得到了N2O分子在NiO(100)表面吸附的两种模型，在这两种构型中，N2O分子和吸附表面是倾斜的，氧端向下和氮端向下的吸附能分别为-9.2190eV和-8.0767eV。相比于离NiO(100)表面的初始距离1.3?，优化后的构型中N2O分子与NiO(100)表面的距离为3.352?、3.732?，这表明N2O在NiO表面的吸附是一个物理吸附过程。关键词：N2O脱除，DFT，NiO(100)表面ABSTRACTN2O is a kind of greenhouse gas which can cause great damage to the atmosphere. It has a strong ability to absorb infrared radiation and lead to global warming.In recent years,with growing awareness of environmental protection,N2O removal technology has been paid more and more attention by researchers in the field of environmental protection.Due to its low reaction temperature without reducing agent,low operating costs, and the harmless resulting decomposition products N2 and O2,direct catalytic decompositionhas become the most promising technology in terms of N2O removal.Studies have shown that NiO, as a metal oxide catalyst, has high efficiency of N2Odecomposition.We use density functional theory (DFT) and CASTEP module of Materials Studio construct NiO(100) surface.We use its DMol3 module discuss the mechanism of N2O decomposition on NiO(100) surface with PBE density function and generalized gradient approximation(GGA) for geometry opitimization based on quantum chemistry theory. Two adsorption models of N2O decomposition on NiO(100) surface are found by transition state search function of DMol3 module,the N2O molecular is inclined with the adsorption surface,the adsorption energy of O down configuration and N down configuration are -9.2190eV and -8.0767eV respectively.Compared with the initial distance between N2O molecular and NiO(100) surface 1.3?, the optimized N2O molecule’s distance are 3.352? and 3.732? r