摘要
采用密度泛函理论方法计算研究了H_(2)分子在MnO_(2)的活化,发现“Mn-O”酸碱对之间的距离对分子的活化起着重要的作用:“Mn-O”键距离越远,活化程度越强,并且在“Mn-O”距离约为0.4 nm作用最强(即形成了表面“受阻路易斯酸碱对”).通过对[H…H]^(≠)过渡态的电子结构性质及相互作用能的分析发现,可以形成“受阻路易斯酸碱对”的“Mn-O活性对”具有最大的整体相互作用能,稳定了过渡态结构.该研究结果有助于人们理解“受阻路易斯酸碱对”协同作用的本质,从而更好地通过调控催化剂的微结构来构筑高活性的“受阻路易斯酸碱对”.
The activation of H_(2) on MnO_(2) is studied by density functional theory calculation,in which it is found that the distance of“Mn-O”plays a key role for the activation of H_(2),that is,the longer the Mn-O distance,the more activation of H_(2),and the most activation occurs at the 0.4 nm(i.e.,a“Frustrated Lewis acid-base pair”is formed).Through the analysis of the electronic structure properties and interaction of the[H…H]^(≠) transition state(TSs),it is found the“Mn-O active pair”that can form a“Frustrated Lewis acid-base pair”has the largest overall interaction energy and thus stabilizes the TSs.The present results may help people to understand the nature of the synergistic effect of the“Frustrated Lewis acid-base pair”,and construct a highly active“Frustrated Lewis acid-base pair”by adjusting the microstructure of the catalyst more efficiently.
作者
王贵昌
WANG Guichang(College of Chemistry,Nankai University,Tianjin 300071,China)
出处
《信阳师范学院学报（自然科学版）》
CAS
北大核心
2021年第4期555-559,共5页
Journal of Xinyang Normal University(Natural Science Edition)
基金
国家自然科学基金项目(21973048)。
