Predicting H2S Oxidative Dehydrogenation over Graphene Oxides from First Principles  

H2S在氧化石墨烯表面的吸附和分解的理论研究

作　　者：黄斌[1] 陈碧波[1] 陈荣[1] 

机构地区：[1]东华理工大学材料系,南昌331000

出　　处：《Chinese Journal of Chemical Physics》2015年第2期143-149,I0001,共8页化学物理学报（英文）

基　　金：This work was supported by the National Natu- ral Science Foundation of China （No.21004009） and the Foundation of Jiangxi Educational Committee （No.G J J13447 and No.G J J14485）. We are grateful to High Performance Computer Center of State Key Lab- oratory of Physical Chemistry of Solid Surface （Xiamen University）.

摘　　要：Spin-polarized periodic density functional theory was performed to characterize H2S adsorp- tion and dissociation on graphene oxides （GO） surface. The comprehensive reaction network of H2S oxidation with epoxy and hydroxyl groups of GO was discussed. It is shown that the reduction reaction is mainly governed by epoxide ring opening and hydroxyl hydrogenation which is initiated by H transfer from H2S or its derivatives, hlrthermore, the presence of another OH group at the opposite side relative to the adsorbed H2S activates the oxygen group to facilitate epoxide ring opening and hydroxyl hydrogenation. For H2S interaction with -O and -OH groups adsorption on each side of graphene, the pathway is a favorable reaction path by the introduction of intermediate states, the predicted energy barriers are 3.2 and 10.4 kcal/mol, respectively, the second H transfer is tile rate-determining step in the whole reaction process. In addition, our calculations suggest that both epoxy and hydroxyl groups can enhance tile binding of S to the C-C bonds and the effect of hydroxyl group is more local than that of the epoxy.

关 键 词：First principles H2S ADSORPTION DISSOCIATION 

分 类 号：O[理学]