煅烧石油焦脱除烟气中Hg^0密度泛函理论研究  

Density Functional Theory Study on Calcined Petroleum Coke for Hg^0 Removal From Flue Gas

作　　者：陆遥 刁永发[1] 肖艺 田力 李晓诠 陈晨 LU Yao;DIAO Yong-Fa;XIAO Yi;TIAN Li;LI Xiao-Quan;CHEN Chen(School of Environmental Science and Engineering,Donghua University,Shanghai 201620,China)

机构地区：[1]东华大学环境科学与工程学院

出　　处：《工程热物理学报》2019年第12期2960-2967,共8页Journal of Engineering Thermophysics

基　　金：中央高校基本科研业务费专项资金暨重点项目(No.CUSF-DH-D-2017097,No.17D111308);上海市优秀技术带头人计划项目(No.14XD1424700)

摘　　要：石油焦作为碳基吸附剂脱除燃煤烟气中Hg^0的研究近年来得到发展,本文建立了表征煅烧石油焦表面的四碳环并噻吩饱和簇模型,运用量子化学密度泛函理论B3LYP-D3方法,基于6-31g(d)/lanl2dz混合基组水平,从微观层面研究了煅烧石油焦吸附Hg^0的机理,同时计算了Hg在煅烧石油焦上的吸附能及Mayer键级,并分析了石油焦中噻吩硫在脱汞中的作用。研究结果表明,Hg^0在煅烧石油焦上的吸附以物理吸附为主,噻吩硫对Hg^0的吸附有促进作用。量子化学理论计算是研究煅烧石油焦吸附剂脱除Hg^0机理的一种有效方法。Petroleum coke has been developed to remove Hg^0 in flue gas as a carbon-based adsorbent recently.Novel petroleum coke models with thiophene inside were designed to characterize the surface of calcined petroleum coke.The adsorption of mercury on calcined petroleum coke was investigated by the density functional theory(DFT) B3 LYP-D3 of quantum chemistry and 6-31 g(d)/lanl2 dz basis set.The binding energy and Mayer bond order of the adsorption were calculated and the effect of sulfur in thiophene ring was discussed.The results showed that the adsorption of Hg^0 on calcined petroleum coke was mainly physical adsorption and the sulfur atom in the model enhanced the adsorption.Quantum chemistry calculation is an effective method to study the mechanism of mercury adsorption by calcined petroleum coke.

关 键 词：汞 石油焦 硫 吸附 簇模型 Mayer键级 

分 类 号：TK16[动力工程及工程热物理—热能工程]