Observation of the interaction between Au− and CO2 in Au(CO2)<i>n</i>− anions: Physisorption as the dominant mechanism

Z Zonghui Guo (School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,) S Shihu Du (School of Chemistry and Chemical Engineering, Shandong University 2 , Jinan 250100,) W Wei Huang W Wenbao Zhao H Haiyan Han (School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,) Z Zhi Zhao Y Yongliang Yan Z Zhihui Fan (School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,) R Ruili Shi (School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,) H Hua Xie (State Key Laboratory of Chemical Reaction Dynamics) L Ling Jiang (Optogenetics & Synthetic Biology Interdisciplinary Research Center, Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism, School of Pharmacy, East China University of Science and Technology, 130 Mei Long Road, Shanghai 200237, China)

Abstract

In this study, we investigated the structure and bonding of Au(CO2)n− (n = 2, 3) using photoelectron spectroscopy analysis, quantum chemical calculations, and weak interaction analysis. Quantum chemical calculations revealed that the geometries of the physisorbed structures closely aligned with experimental data, suggesting that these configurations were the most stable under the experimental conditions. Conversely, while chemisorbed structures exhibit stronger interactions and considerable CO2 activation, they show less agreement with the observed spectroscopic data. Using the interaction region indicator method, our weak interaction analysis confirmed that van der Waals forces were the dominant interaction in the physisorbed structures. Our experimental results indicate that these physically adsorbed structures are more stable under the conditions of this study. These findings shed light on the interaction mechanisms of Au(CO2)n− (n = 2, 3) at the molecular level and provide new insights into the potential for transition metals to catalytically activate CO2.

Article Details

Volume / Issue Vol. 162, Issue 17
Published May 07, 2025
ISSN 0021-9606
Publisher American Institute of Physics

Journal Info

The Journal of Chemical Physics

American Institute of Physics

ISSN: 0021-9606 Physical Sciences

Authors (11)

Z

Zonghui Guo

School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,

S

Shihu Du

School of Chemistry and Chemical Engineering, Shandong University 2 , Jinan 250100,

W

Wei Huang

W

Wenbao Zhao

H

Haiyan Han

School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,

Z

Zhi Zhao

Y

Yongliang Yan

Z

Zhihui Fan

School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,

R

Ruili Shi

School of Mathematics and Physics Science and Engineering, Hebei Computational Optical Imaging and Photoelectric Detection Technology Innovation Center, Hebei International Joint Research Center for Computational Optical Imaging and Intelligent Sensing, Hebei University of Engineering 1 , Handan 056038,

H

Hua Xie

State Key Laboratory of Chemical Reaction Dynamics

L

Ling Jiang

Optogenetics & Synthetic Biology Interdisciplinary Research Center, Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism, School of Pharmacy, East China University of Science and Technology, 130 Mei Long Road, Shanghai 200237, China