摘要
本文利用线形飞行时间质谱,在低能量电子与液体甲醇碰撞中探测到了负离子产物.利用量子化学计算,进一步确定负离子产物为氢键结合的分子团簇CH_(3)OH.CH_(3)O^(-)和CH_(3)OH.CH_(3)OH.CH_(3)O^(-),而且其单占据分子轨道表现为价层轨道特征.虽然CH_(3)OH.CH_(3)OH^(-)和CH_(3)OH.CH_(3)OH.CH_(3)OH^(-)对应各自势能面的极小点,但能量上相比脱氢团簇不具有产生优势,且其单占据分子轨道具有显著的溶剂化电子特征.
In the low-energy electron impacts with a liquid beam of methanol,we detect the anionic yields using a linear time-of-flight mass spectrometer.With help of quantum chemistry calculations,we further identify these anionic products as the hydrogenbondingclusters,i.e.,CHgOH·CHgO^(-)and CHgOH·CH:OH·CH_(3)O^(-),and their singly occupied molecular orbitals show the valence-bound feature.In contrast,CH_(3)OH^(-)CH_(3)OH and CH_(3)OH^(-)CH_(3)OH·CH_(3)OH are unfavored in energetics with respect to the dehydrogenated ones,although they also correspond to the minima on the potential energy surfaces.Furthermore,the singly occupied molecular orbitals of CH_(3)OH·CH_(3)OH and CH_(3)OH·CH_(3)OH·CH_(3)OH^(-)indicate the typical feature of aqueous-solvated electron.
作者
陈子伟
李子渊
田善喜
Ziwei Chen;Ziyuan Li;Shan Xi Tian(Department of Chemical Physics,Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes,Collaborative Innovation Center of Chemistry for Energy Materials(iChEM),University of Science and Technology of China,Hefei 230026,China;Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei 230026,China)
基金
supported by the National Natural Science Foundation of China(No.21625301)。
关键词
负离子团簇
低能量电子
液体束
Anionic cluster
Low-energy electron
Liquid beam
