密度泛函理论研究NO在CuO(1 1 1)的表面吸附  

Study of NO Adsorption on CuO(1 1 1) Surface by Density Functional Theory

作　　者：杨秀荣 张驰[1] 高红旭[2] 赵凤起[2] 牛诗尧 马海霞[1] YANG Xiu-rong;ZHANG Chi;GAO Hong-xu;ZHAO Feng-qi;NIU Shi-yao;MA Hai-xia(School of Chemical Engineering,Northwest University,Xi′an 710069,China;Science and Technology on Combustion and Explosion Laboratory,Xi′an Modern Chemistry Research Institute,Xi′an 710065,China)

机构地区：[1]西北大学化工学院,陕西西安710069 [2]西安近代化学研究所燃烧与爆炸技术重点实验室,陕西西安710065

出　　处：《火炸药学报》2019年第2期125-130,190,I0002,共8页Chinese Journal of Explosives & Propellants

基　　金：国家自然科学基金(No.21673179;No.21504067;No.21373161);预研领域基金资助(No.6140656020216BQ34001)

摘　　要：为了深入研究纳米CuO与含能材料分解产生的NO间的相互作用,采用密度泛函理论研究了NO在CuO(1 1 1)表面的吸附行为,同时在NO吸附的最稳定位点研究NO_2在Cu表面的吸附及其对NO的影响;通过DMol^3模块中广义梯度密度泛函理论(GGA)的Perdew-Burke-Ernzerh (PBE)方法对吸附构型进行了计算。结果表明,NO以分子形式吸附在CuO(1 1 1)表面,较为稳定的吸附构型为NO的N原子与CuO表面的Cu、O原子相互作用,均为化学吸附;最稳定的吸附构型为NO吸附在Cu1位点上,吸附能为-0.89eV;HOMO-LUMO轨道能隙值和态密度图分析均表明NO和CuO表面有强烈相互作用;Mulliken电荷布局分析显示,电荷从NO转移到Cu表面,NO带部分正电荷;在含能材料分解过程中,NO气体稳定吸附在CuO表面,但当存在NO_2时,NO的吸附位点可能会被吸附能力更强的NO_2占据。To deeply study the interaction between nano CuO and NO produced by the decomposition of energetic materials(EMs),the adsorption behavior of NO on CuO(1 1 1)surface was investigated using density functional theory and at the most stable point of NO adsorption,the adsorption of NO2 on the surface of Cu surface and its influence on NO were studied.The adsorption configuration was calculated by the Perdew-Burke-Ernzerh(PBE)method of generalized gradient approximation(GGA)in DMol3 module.The results show that NO is adsorbed on the surface of CuO(1 1 1)in molecular form.The stable adsorption configuration is that the nitrogen atoms of NO interacts with the oxygen and copper atoms on the surface of CuO and all of them are chemical adsorption.The most stable adsorption configuration is that NO is adsorbed on Cu1 site and the adsorption energy is-0.89eV.The analysis of the HOMO-LUMO gaps and density of states indicate that there is a strong interaction between NO and CuO surface.Mulliken charge analysis shows that the charge transfers from NO to Cu surface,thus NO has a partial positive charge.In the decomposition process of EMs,NO gas is stably adsorbed on the surface of CuO,but the adsorption sites of NO may be occupied when there is NO2 which has a stronger adsorption ability.

关 键 词：量子化学 密度泛函理论 纳米CUO NO 吸附 

分 类 号：TJ55[兵器科学与技术—军事化学与烟火技术] O641[理学—物理化学]