DFT study on the regeneration mechanism of ZnO surface during the desulfurization of H2S

被引：15

作者：

Ling, Lixia ^{[1
,2
]}

Han, Peide ^{[2
]}

Wang, Baojun ^{[3
]}

Zhang, Riguang ^{[3
]}

机构：

[1] Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China

[2] Taiyuan Univ Technol, Coll Mat Sci & Engn, Taiyuan 030024, Shanxi, Peoples R China

[3] Taiyuan Univ Technol, Minist Educ & Shanxi Prov, Key Lab Coal Sci & Technol, Taiyuan 030024, Shanxi, Peoples R China

来源：

FUEL PROCESSING TECHNOLOGY | 2013年 / 109卷

基金：

中国国家自然科学基金;

关键词：

Regeneration mechanism; Sulfurized surface; Oxygen-deficient surface; Density functional theory; GENERALIZED GRADIENT APPROXIMATION; AB-INITIO; ADSORPTION; REMOVAL; 10(1)OVER-BAR0; SORBENTS; O-2;

D O I：

10.1016/j.fuproc.2012.09.037

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

The regeneration mechanisms of the sulfurized and oxygen-deficient ZnO(10 (1) over bar0) surfaces in an oxygen atmosphere have been systematically studied by using the density functional theory (OFF) method. An activation energy of 36.79 kJ.mol(-1) is needed for the regeneration of the sulfurized ZnO(10 (1) over bar0) surface at the GGA-PW91 functional level. The formed SO2 lies on the ZnO(10 (1) over bar0) surface horizontally. S in SO2 bonds to a surface oxygen atom to form an analogical SO3 structure. Two regeneration mechanisms are studied for the oxygen-deficient ZnO(10 (1) over bar0) surface. One is that O-2 dissociatively adsorbs on the oxygen-deficient ZnO(10 (1) over bar0) surface leading to the regeneration of the surface. The other is that O-2 molecularly adsorbs on the oxygen-deficient ZnO(10 (1) over bar0) surface, then a little activation energy of 29.43 kJ.mol(-1) is needed to make the surface regenerate. It can be concluded that the sulfurized and oxygen-deficient ZnO(10 (1) over bar0) surfaces are easy to be regenerated in an atmosphere containing O-2. (c) 2012 Elsevier B.V. All rights reserved.

引用

页码：49 / 56

页数：8

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