The adsorption of CO2, H2CO3, HCO3-and CO32-on Cu2O (111) surface: First-principles study

被引：30

作者：

Wu, Huanwen ^{[1
]}

Zhang, Ning ^{[1
]}

Cao, Zhiji ^{[2
]}

Wang, Hongming ^{[1
]}

Hong, Sanguo ^{[1
]}

机构：

[1] Nanchang Univ, Dept Chem, Nanchang 330031, Jiangxi, Peoples R China

[2] Calif State Univ Hayward, Dept Math & Comp Sci, Hayward, CA 94542 USA

来源：

INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY | 2012年 / 112卷 / 12期

关键词：

Cu2O (111); surface; carbon dioxide species; bicarbonate ion; adsorption; First-principles calculation; ORBITAL CLUSTER MODEL; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; AB-INITIO; ELECTROLYTIC REDUCTION; AQUEOUS-SOLUTION; ACTIVE-SITES; BICARBONATE; WATER; ELECTROREDUCTION;

D O I：

10.1002/qua.23250

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：

The adsorption of CO2, and its derivatives, H2CO3, HCO3-, and CO?32-, on Cu2O (111) surface has been investigated by first-principles calculations based on the density functional theory at B3LYP hybrid functional level. The Cu2O (111) surface has been modeled using an embedded cluster method,in which the quantum clusters plus some ab initio ion model potentials were inserted in an array of point charges. On the surface, H2CO3 was dissociated into an H+ and an HCO?3- ion. Among the CO2 species, HCO?3- was the only activated species on the surface. The results suggest that the reduction of CO2 on Cu2O (111) surface can start from the form of HCO?3-. (C) 2011 Wiley Periodicals, Inc. Int J Quantum Chem, 2011

引用

页码：2532 / 2540

页数：9

共 65 条

[51] ELECTRONIC-STRUCTURES OF ACTIVE-SITES ON METAL-OXIDE SURFACES - DEFINITION OF THE CU/ZNO METHANOL SYNTHESIS CATALYST BY PHOTOELECTRON-SPECTROSCOPY [J].

SOLOMON, EI ;

JONES, PM ;

MAY, JA .

CHEMICAL REVIEWS, 1993, 93 (08) :2623-2644

[52] Plane-wave pseudopotential density functional theory periodic slab calculations of CO adsorption on Cu2O(111) surface [J].

Soon, A ;

Söhnel, T ;

Idriss, H .

SURFACE SCIENCE, 2005, 579 (2-3) :131-140

[53] SUPPORTED PALLADIUM CATALYSTS FOR THE REDUCTION OF SODIUM-BICARBONATE TO SODIUM FORMATE IN AQUEOUS-SOLUTION AT ROOM-TEMPERATURE AND ONE ATMOSPHERE OF HYDROGEN [J].

STALDER, CJ ;

CHAO, S ;

SUMMERS, DP ;

WRIGHTON, MS .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1983, 105 (20) :6318-6320

[54] ELECTROCHEMICAL REDUCTION OF AQUEOUS BICARBONATE TO FORMATE WITH HIGH-CURRENT EFFICIENCY NEAR THE THERMODYNAMIC POTENTIAL AT CHEMICALLY DERIVATIZED ELECTRODES [J].

STALDER, CJ ;

CHAO, S ;

WRIGHTON, MS .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1984, 106 (12) :3673-3675

[55] SELECTIVE PHOTOREDUCTION OF CARBON-DIOXIDE TO METHANOL WITH HYDROUS CUPROUS-OXIDE [J].

TENNAKONE, K ;

JAYATISSA, AH ;

PUNCHIHEWA, S .

JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 1989, 49 (03) :369-375

[56] Relationship between hydrocarbon production in the electrochemical reduction of CO2 and the characteristics of the Cu electrode [J].

Terunuma, Y ;

Saitoh, A ;

Momose, Y .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1997, 434 (1-2) :69-75

[57] POTENTIAL-ENERGY SURFACE AND VIBRATIONAL FREQUENCIES OF CARBONIC-ACID [J].

WIGHT, CA ;

BOLDYREV, AI .

JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (32) :12125-12130

[58] Hybrid density functional theory study of the high-pressure polymorphs of α-Fe2O3 hematite [J].

Wilson, Nicholas C. ;

Russo, Salvy P. .

PHYSICAL REVIEW B, 2009, 79 (09)

[59] THEORETICAL-STUDY OF A CU+ ION IMPURITY IN A NAF HOST [J].

WINTER, NW ;

PITZER, RM ;

TEMPLE, DK .

JOURNAL OF CHEMICAL PHYSICS, 1987, 86 (06) :3549-3556

[60] Photocatalytic Reduction of Greenhouse Gas CO2 to Fuel [J].

Wu, Jeffrey C. S. .

CATALYSIS SURVEYS FROM ASIA, 2009, 13 (01) :30-40

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