H2O影响γ-Al2O3吸附SO2、NO的机理分析  

MECHANISM ANALYSIS OF EFFECT OF H2O ON ADSORPTION OF SO2 AND NO ON γ-Al2O3

作　　者：华腾云 张晨昕[1] 武传朋 郭大为[1] 毛安国[1] Hua Tengyun;Zhang Chenxin;Wu Chuanpeng;Guo Dawei;Mao Anguo(SINOPEC Research Institute of Petroleum Processing,Beijing 100083;CNPC EastChina Design Institute Co.Ltd.)

机构地区：[1]中国石化石油化工科学研究院,北京100083 [2]中石油华东设计院有限公司

出　　处：《石油炼制与化工》2020年第2期50-56,共7页Petroleum Processing and Petrochemicals

基　　金：国家自然科学基金项目(U21576096);中国石油化工股份有限公司合同项目(S118001-9)

摘　　要：利用分子模拟与实验探究结合,考察了H2O影响γ-Al2O3吸附SO2、NO的机理。在构造γ-Al2O3(110C)面基础模型和建立H2O,SO2,NO等吸附质分子在(110C)面的吸附模型后,确定了优化的吸附构象。通过电荷密度和分波态密度分析发现,吸附质与(110C)面Al位点存在明显的电子转移,进而形成稳定的吸附结构。H2O通过分子吸附和解离吸附,占据Al3c和O3c位点;SO2主要吸附在Al3c、Al4c位点;NO与Al4c位点相互作用,需要在O3c位点氧化。因此,H2O与SO2和NO在γ-Al2O3(110C)面的Al3c和O3c位点存在竞争吸附。试验结果与分子模拟理论分析结果基本一致,H2O不利于SO2和NO在γ-Al2O3上的吸附。The mechanism of the influence of H2O on the adsorption of SO2 and NO onγ-Al2O3 was investigated by molecular simulation and experimental investigation.The adsorption structure ofγ-Al2O3(110C)surface was constructed,and the adsorption models for H2O,SO2,NO molecules on(110C)surface were established to determine the optimized adsorption structure.It was found that there was obvious electron transfer between adsorbate and(110C)Al site by charge density and partial density of states,resulting in the formation of stable adsorption structure.H2O occupied Al3c and O3c sites through molecular adsorption and dissociation adsorption;SO2 was mainly adsorbed at Al3c and Al4c sites,while NO interacted with the Al4c sites and needed to be oxidized at the O3c sites.Therefore,there is a competitive adsorption among H2O,SO2,NO at Al3c and O3c sites on theγ-Al2O3(110C)surface.The experimental results were basically consistent with the theoretical analysis of molecular simulation.H2O is not conducive to the adsorption of SO2 and NO onγ-Al2O3.

关 键 词：分子模拟 水 氧化铝 二氧化硫 一氧化氮 

分 类 号：O64[理学—物理化学]