钙元素对焦炭表面NO吸附行为的影响-密度泛函理论研究.pdfVIP

第43卷 第12期 燃 料 化 学 学 报 Vol.43 No.12 2015年12月 Journal of Fuel Chemistry and Technology Dec. 2015 文章编号:0253-2409(2015)12-1414-06 钙元素对焦炭表面NO 吸附行为的影响:密度泛函理论研究 * 刘 磊,金 晶 ,林郁郁,侯封校 (上海理工大学 能源与动力工程学院,上海 200093) 摘 要:采用密度泛函理论研究了Ca元素对焦炭表面NO吸附行为的影响。 使用周期性石墨烯模型近似模拟实际焦炭表面 的石墨化结构,并在石墨烯表面装饰Ca原子(按质量计Ca原子覆盖率为13.3%),考察了Ca元素对焦炭表面NO 吸附的催 化作用。 计算结果表明,NO分子在纯净石墨烯表面的吸附属于物理吸附,结合能仅为-19.34kJ/ mol;石墨烯表面掺入Ca原 子后,由于Ca原子4s轨道和3d轨道的电子转移到NO分子,结合能显著提高至-206.02kJ/ mol。 关键词:焦炭;一氧化氮;钙;吸附;密度泛函理论 中图分类号:TK16 文献标识码:A Effect of calcium on the absorption of NO on char surface: A density functional theory study * LIU Lei,JIN Jing ,LIN Yu-yu,HOU Feng-xiao (Department of Energy and PowerEngineering,University of ShanghaiforScience and Technology,Shanghai 200093,China) Abstract:The effectofcalciumontheadsorptionofNOonchar surfacewasstudiedbyusingdensityfunctional theory. Periodic boundary graphene model was adopted to simulate the graphitic structure of char surface;the catalytic effect of calcium on NO adsorption was investigated by decorating the graphene surface with calcium atomswhich have a coverage rate of 13.3%. The results demonstrated that NO is physically adsorbed on the pristine graphene surface,with a binding energy of -19.34 kJ/ mol;after decorating the graphene surface with calcium atoms,the adsorption isturned into a chemical sorption with a binding energy of -206.02kJ/ mol,due to the transfer of electronsin4s and3d orbitals of Ca atom to the NO molecule. Key words:char;nitric oxide;calcium;adsorption;density functional theory 燃煤电厂排放的烟气中通常含有大量氮氧化物 学的手段系统地研究了NO 和N O在多元碳环模