First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO2(111) and CeO2(110) surfaces

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (3): 524-532.

First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO₂(111) and CeO₂(110) surfaces

Donghai Mei

Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, Washington 99352, USA

收稿日期:2012-12-11 修回日期:2013-01-16 出版日期:2013-05-20 发布日期:2013-05-31
通讯作者: Donghai Mei
基金资助:
This work was supported by the Laboratory Directed Research and Development (LDRD) Project of the Pacific Northwest National Laboratory (PNNL). The computations were performed using the Molecular Science Computing Facility in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), which is a U. S. Department of Energy national scientific user facility located at PNNL in Richland, Washington. Part of the computing time was also granted by the National Energy Research Scientific Computing Center (NERSC).

First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO₂(111) and CeO₂(110) surfaces

Donghai Mei

Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, Washington 99352, USA

Received:2012-12-11 Revised:2013-01-16 Online:2013-05-20 Published:2013-05-31
Supported by:
This work was supported by the Laboratory Directed Research and Development (LDRD) Project of the Pacific Northwest National Laboratory (PNNL). The computations were performed using the Molecular Science Computing Facility in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), which is a U. S. Department of Energy national scientific user facility located at PNNL in Richland, Washington. Part of the computing time was also granted by the National Energy Research Scientific Computing Center (NERSC).

摘要/Abstract

摘要： Molecular adsorption of formate and carboxyl on stoichiometric CeO₂(111) and CeO₂(110) surfaces was studied using periodic density functional theory (DFT+U) calculations. Two distinguishable adsorption modes (strong and weak) of formate are identified. The bidentate configuration is more stable than the monodentate adsorption configuration. Both formate and carboxyl bind at the more open CeO₂(110) surface are stronger. The calculated vibrational frequencies of two adsorbed species are consistent with the experimental measurements. Finally, the effects of U parameters on the adsorption of formate and carboxyl over both CeO₂ surfaces were investigated. We found that the geometrical configurations of two adsorbed species are not affected by different U parameters (U = 0, 5, and 7). However, the calculated adsorption energy of carboxyl pronouncedly increases with the U value while the adsorption energy of formate only slightly changes (<0.2 eV). The Bader charge analysis shows the opposite charge transfer occurs for formate and carboxyl adsorption where the adsorbed formate is negatively charge while the adsorbed carboxyl is positively charged. Interestingly, with the increasing U parameter, the amount of charge is also increased.

关键词: cerium oxide, adsorption, formate, carboxyl, density functional theory

Abstract: Molecular adsorption of formate and carboxyl on stoichiometric CeO₂(111) and CeO₂(110) surfaces was studied using periodic density functional theory (DFT+U) calculations. Two distinguishable adsorption modes (strong and weak) of formate are identified. The bidentate configuration is more stable than the monodentate adsorption configuration. Both formate and carboxyl bind at the more open CeO₂(110) surface are stronger. The calculated vibrational frequencies of two adsorbed species are consistent with the experimental measurements. Finally, the effects of U parameters on the adsorption of formate and carboxyl over both CeO₂ surfaces were investigated. We found that the geometrical configurations of two adsorbed species are not affected by different U parameters (U = 0, 5, and 7). However, the calculated adsorption energy of carboxyl pronouncedly increases with the U value while the adsorption energy of formate only slightly changes (<0.2 eV). The Bader charge analysis shows the opposite charge transfer occurs for formate and carboxyl adsorption where the adsorbed formate is negatively charge while the adsorbed carboxyl is positively charged. Interestingly, with the increasing U parameter, the amount of charge is also increased.

Key words: cerium oxide, adsorption, formate, carboxyl, density functional theory

Donghai Mei. First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO₂(111) and CeO₂(110) surfaces[J]. 能源化学(英文), 2013, 22(3): 524-532.

Donghai Mei. First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO₂(111) and CeO₂(110) surfaces[J]. Journal of Energy Chemistry, 2013, 22(3): 524-532.

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First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO₂(111) and CeO₂(110) surfaces

First-principles characterization of formate and carboxyl adsorption on stoichiometric CeO₂(111) and CeO₂(110) surfaces

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