Prediction of structural and electronic properties of Cl2 adsorbed on TiO2(100)surface with C or CO in fluidized chlorination process:A first-principles study  

沸腾氯化过程中C和CO分别与Cl2在TiO2(100)表面的吸附结构及电荷属性分析:第一性原理研究

作　　者：YANG Fan WEN Liang-ying PENG Qin ZHAO Yan XU Jian HU Mei-long ZHANG Sheng-fu YANG Zhong-qing 杨帆;温良英;彭琴;赵岩;徐健;扈玫珑;张生富;杨仲卿(School of Materials Science and Engineering,Chongqing University,Chongqing 400044,China;Chongqing Key Laboratory of Vanadium-Titanium Metallurgy and Advanced Materials,Chongqing University,Chongqing 400044,China;School of Power Engineering,Chongqing University,Chongqing 400044,China)

机构地区：[1]School of Materials Science and Engineering,Chongqing University,Chongqing 400044,China [2]Chongqing Key Laboratory of Vanadium-Titanium Metallurgy and Advanced Materials,Chongqing University,Chongqing 400044,China [3]School of Power Engineering,Chongqing University,Chongqing 400044,China

出　　处：《Journal of Central South University》2021年第1期29-38,共10页中南大学学报（英文版）

基　　金：Projects(51674052,51974046)supported by the National Natural Science Foundation of China;Project(cstc2018jcyjAX0003)supported by the Chongqing Research Program of Basic Research and Frontier Technology,China。

摘　　要：Based on the first-principles calculations of density functional theory,co-adsorption models of C or CO with Cl2 on rutile TiO2(100)surface were established.The adsorption structures and electronic properties during chlorination process were predicted.Then,the adsorption energy,charge density,electron density difference and density of state of the adsorption structures were calculated and analyzed.The stabilities of the adsorption structures and the charge distributions between atoms were studied.It was found that both C and CO could promote the adsorption reactions of Cl2 on TiO2(100)surface,and C was more favorable to the adsorption process.The results show that the adsorption process of Cl2 on TiO2(100)surface was physisorption,and the co-adsorption processes of C or CO with Cl2 on TiO2(100)surface were chemisorptions.基于密度泛函理论的第一性原理计算方法,构建C和CO分别与Cl2在金红石TiO2(100)面共吸附模型,预测了氯化过程中的吸附结构及其电荷属性。之后,对吸附结构的吸附能、电荷密度、差分电荷密度和态密度等进行计算分析,研究了吸附结构的稳定性及原子间的电荷分布。发现C和CO均能促使Cl2在TiO2(100)表面发生吸附反应,且C更有利于促进吸附反应的发生。结果表明:Cl2分子单独在TiO2(100)表面吸附的过程为物理吸附,C和CO分别与Cl2同时在TiO2(100)表面吸附的过程均为化学吸附。

关 键 词：FIRST-PRINCIPLES co-adsorption model titanium dioxide BONDING 

分 类 号：TQ134.11[化学工程—无机化工] O647.31[理学—物理化学]