Surface property of the Cu doped γ-Al2O3: A density functional theory study

被引:23
作者
Shi, Liu [1 ]
Huang, Yan [1 ]
Lu, Zhang-Hui [2 ]
Cen, Wanglai [3 ]
Yu, Xiaohu [4 ,5 ,6 ]
Qing, Shaojun [7 ]
Gao, Zhixian [7 ]
Zhang, Rongbin [1 ]
Feng, Gang [1 ]
机构
[1] Nanchang Univ, Coll Chem, Inst Appl Chem, Key Lab Jiangxi Prov Environm & Energy Catalysis, 999Xuefu Rd, Nanchang 330031, Jiangxi, Peoples R China
[2] Jiangxi Normal Univ, Coll Chem & Chem Engn, Inst Adv Mat IAM, Nanchang 330022, Jiangxi, Peoples R China
[3] Sichuan Univ, Inst New Energy & Low Carbon Technol, Chengdu 610065, Peoples R China
[4] Shaanxi Univ Technol, Sch Chem & Environm Sci, Inst Theoret & Computat Chem, Shaanxi Key Lab Catalysis, Hanshong 723000, Peoples R China
[5] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[6] Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China
[7] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
基金
中国国家自然科学基金;
关键词
Cu/gamma-A1(2)O(3); Substitution; Density functional theory; Dehydration; Surface property; TOTAL-ENERGY CALCULATIONS; N N=1-4 CLUSTERS; SPECTROSCOPIC CHARACTERIZATION; CU/GAMMA-AL2O3; CATALYST; METHANOL SYNTHESIS; CO2; HYDROGENATION; COPPER ALUMINATE; GAMMA-ALUMINA; CU/AL2O3; ADSORPTION;
D O I
10.1016/j.apsusc.2020.147651
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Cu/gamma-Al2O3 catalysts are widely used in many catalytic processes. Investigation into the catalysts structure at molecular level is the basis for the elucidation of the reaction mechanisms and favors the developments of the catalysts. In the present work, periodic density functional theory calculations were performed to investigate the interface of alumina with copper oxides. The interface model is chosen as the substitution of the surface Al atoms of gamma-Al2O3 with Cu, and H is used as the ion for charge balance. It is found that the substitution of surface Al a by Cu2+ is thermodynamically accessible. Gibbs free energy calculations show that the dehydration temperature for the gamma-Al2O3 (1 1 0) surface after substitution is higher than that of on the original gamma-Al2O3 (1 1 0) and CuAl2O4 surface. The oxygen vacancy formation energies for the (1 0 0)-5Cu-dehy-2w and (1 1 0)-4Cu-dehy-2w are 213 and 367 kJ/mol, respectively. In addition, the Cu doped-gamma-Al2O3 interface could strengthen the binding of Cu with the alumina surface. The results provide molecular level insights for the understanding of the interface structures and physical chemistry properties of alumina with copper oxides.
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页数:11
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