五角石墨烯吸附H_(2)S的第一性原理计算

First principles calculation of adsorption of hydrogen sulfide on pentagonal graphene

硫化氢作为一种神经毒物和腐蚀性气体污染物,严重威胁人体健康并限制工业的发展.本文采用第一性原理计算的方法,研究了H_(2)S气体分子在原始五角石墨烯、非金属掺杂及金属掺杂五角石墨烯上的吸附行为.详细计算了H_(2)S气体分子与五角石墨烯之间的吸附构型、吸附能及电荷转移.结果表明:1)原始五角石墨烯和非金属元素掺杂五角石墨烯与H_(2)S气体分子间仅为微弱的物理吸附,无法直接用于吸附H_(2)S气体;2) Co、Ni、Cu及Ti掺杂的五角石墨烯对H_(2)S气体的吸附作用显著增强.当金属掺杂在sp^(2)C位置时,掺杂五角石墨烯对H_(2)S气体的吸附效果较好,此时的吸附均为化学吸附;3) Co、Ni、Cu及Ti掺杂的五角石墨烯均可作为H_(2)S气体的传感/捕获材料.其中Cu掺杂五角石墨烯吸附H_(2)S气体的效果最好.本文的研究结果对设计开发基于五角石墨烯的H_(2)S气体传感/捕获材料提供了理论指导.

As a neurotoxic and corrosive gas pollutant, hydrogen sulfide poses a serious threat to human health and limits the development of industry. In this paper, the adsorption behavior of H_(2)S gas molecules on the original pentagonal graphene, nonmetal doped graphene and metal doped pentagonal graphene was studied by first principles calculation. The adsorption configuration, adsorption energy and charge transfer between H_(2)S and graphene were calculated in detail. The results show that: 1) there is only weak physical adsorption between the original pentagonal graphene and non-metallic elements doped graphene and H_(2)S gas molecules, while cannot be directly used to adsorb H_(2)S gas. 2) The adsorption of H_(2)S gas on pentagonal graphene doped with Co、Ni、Cu and Ti was significantly enhanced. When the metal atom doped at the sp^(2)C position, the adsorption effect of the doped pentagonal graphene on H_(2)S was better, and the adsorption in this condition belongs to chemical adsorption. 3) Co、Ni、Cu and Ti doped pentagonal graphene can be used as H_(2)S gas sensing/trapping materials. Among them, Cu-doped pentagonal graphene has the best adsorption effect on H_(2)S gas. It is hoped that the research result in this paper can provide theoretical guidance for the design and development of hydrogen sulfide gas sensing/trapping materials based on pentagonal graphene.