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Frontier Molecular Orbital Based Analysis of Solid-Adsorbate Interactions over Group 13 Metal Oxide Surfaces
| Title: | Frontier Molecular Orbital Based Analysis of Solid-Adsorbate Interactions over Group 13 Metal Oxide Surfaces |
| Authors: | Liu, Chong Browse this author | | Li, Yuxin Browse this author | | Takao, Motoshi Browse this author | | Toyao, Takashi Browse this author →KAKEN DB | | Maeno, Zen Browse this author →KAKEN DB | | Kamachi, Takashi Browse this author | | Hinuma, Yoyo Browse this author | | Takigawa, Ichigaku Browse this author →KAKEN DB | | Shimizu, Ken-ichi Browse this author →KAKEN DB |
| Issue Date: | 16-Jul-2020 |
| Publisher: | American Chemical Society |
| Journal Title: | Journal of physical chemistry c |
| Volume: | 124 |
| Issue: | 28 |
| Start Page: | 15355 |
| End Page: | 15365 |
| Publisher DOI: | 10.1021/acs.jpcc.0c04480 |
| Abstract: | Adsorption is an essential process that takes place in heterogeneous catalysis. In the current study, solid-adsorbate interactions occurring between a variety of small molecules and surfaces of group beta metal oxides, including beta-Ga2O3(100), beta-Ga2O3(001), theta-Al2O3 (100), theta-Al2O3 (001), theta-Al2O3 (010), In2O3(110), and In2O3(111), were investigated using density functional theory calculations and a machine learning (ML)-based statistical method. The adsorbates utilized for this purpose include CO, CO2, ND NH3, H2O, acetonitrile, acetone, acetamide, acetic acid, alkanes, alkenes, aromatic compounds, alcohols, and amines. The results show that the adsorption energies (E-ads) of each metal oxide surface correlate linearly with the highest occupied molecular orbital (HOMO) energies of the adsorbates and not with energies of the lowest unoccupied molecular orbital (LUMO) of the small molecules. Moreover, in these systems, contributions to molecular adsorption are dominated by interactions between the HOMOs of the adsorbates and the surface conduction band of the metal oxides. Furthermore, the surface energy was found to be an important parameter influencing E-ads values of different metal oxides. Finally, the results of statistical analysis using a ML approach confirmed that adsorbate HOMOs and surface energy of metal oxides are the most influential factors governing molecular adsorption, and also demonstrated that dipole moments of adsorbates contribute to controlling to adsorption. |
| Rights: | This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpcc.0c04480 . |
| Type: | article (author version) |
| URI: | http://hdl.handle.net/2115/82235 |
| Appears in Collections: | 触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)
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Submitter: 鳥屋尾 隆
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