含氢空位氢化金刚石2维原子晶体体系与硫酸吲哚酚和水分子相互作用的第一性原理计算  

First-principles study on interactions between hydrogenated two-dimensional atomic diamonds with hydrogen vacancy and indoxyl sulfate and water molecules

作　　者：耿俊杰 张兆春[1] 鄢奇桢 郭海波 王洋[2] GENG Junjie;ZHANG Zhaochun;YAN Qizhen;GUO Haibo;WANG Yang(School of Materials Science and Engineering,Shanghai University,Shanghai 200444,China;School of Computer Engineering and Science,Shanghai University,Shanghai 200444,China)

机构地区：[1]上海大学材料科学与工程学院,上海200444 [2]上海大学计算机工程与科学学院,上海200444

出　　处：《上海大学学报（自然科学版）》2023年第2期277-286,共10页Journal of Shanghai University:Natural Science Edition

摘　　要：基于立方金刚石晶体结构构建了2种2维原子晶体:氢化立方金刚石(hydrogenated cubic diamond,HCD)和含氢空位氢化立方金刚石(hydrogen vacancy-HCD,Hv-HCD);将含氢空位氢化立方金刚石与单层六方氮化硼(h-BN)和石墨烯(graphene,G)组装构建了2种2维原子晶体范德华异质结构:h-BN/Hv-HCD和G/Hv-HCD.根据第一性原理,对含氢空位氢化立方金刚石2维原子晶体体系、硫酸吲哚酚和水分子的Fukui函数进行了计算.研究结果显示,含氢空位氢化立方金刚石2维原子晶体体系的氢空位碳原子具有较大的f+(r)和f-(r)值,表明氢空位碳原子的亲电和亲核反应趋势较为显著.有关能量效应的计算结果表明:水分子与含氢空位氢化立方金刚石2维原子晶体体系的氢空位碳原子形成氢键;硫酸吲哚酚分子在氢空位碳原子位点发生化学分解,生成3-吲哚酮和二氧化硫,原磺酸基羟基与氢空位碳原子结合形成醇羟基.该体系可以作为基于2维原子晶体研发生物活性分子、人体血液毒素分子吸附清除以及检测分析核心材料的参考依据.The aim of this study was to construct hydrogenated two-dimensional cu-bic atomic diamonds with hydrogen vacancy-hydrogenated cubic diamond(Hv-HCD)and without hydrogen vacancy(HCD).Furthermore,the isolated monolayer of hexagonal boron nitride(h-BN)or graphene(G)and Hv-HCD were reassembled into van de Waals het-erostructures,h-BN/Hv-HCD,and G/Hv-HCD.Based onfirst-principles,the Fukui func-tions of water,indoxyl sulfate,and the constructed hydrogenated two-dimensional cubic atomic diamonds with hydrogen vacancy were calculated.The largest values of f+(r)and f−(r)lie around the carbon atom close to the hydrogen vacancy,implying that the carbon atom was the nucleophilic and electrophilic reactive site.The results indicate that a water molecule forms a hydrogen bond with the carbon atom close to the hydrogen vacancy of the hydrogenated two-dimensional atomic diamonds with hydrogen vacancy.The indoxyl phosphate molecule is degraded into 3-indolone and sulfur dioxide at the carbon atom close to the hydrogen vacancy site.The hydroxyl in the sulfonic group forms an alcoholic hy-droxyl with the carbon atom close to the hydrogen vacancy.The phenomena described here could provide a foundation for investigating the essential materials for the development of bioactive or human blood toxic molecule sensors based on two-dimensional atomic crystals.

关 键 词：氢空位 2维原子晶体 硫酸吲哚酚 水分子 Fukui函数 

分 类 号：O561[理学—原子与分子物理]