Excitonic Effects of the Excited-State Photocatalytic Reaction at the Molecule/Metal Oxide Interface

Wang, Lei1,2; Liu, Xiaofeng3; Wan, Lingyun4,5; Gao, Yunzhi4,5; Wang, Xiaoning1,2; Liu, Jie4,5; Tan, Shijing4,5; Guo, Qing6; Zhao, Wenhui7; Hu, Wei4,5; Li, Qunxiang1,2; Yang, Jinlong1,2

2024-02-15

10.1021/acs.jpclett.3c03075

JOURNAL OF PHYSICAL CHEMISTRY LETTERS   影响因子和分区

1948-7185

Excitonic effects caused by the Coulomb interaction between electrons and holes play a crucial role in photocatalysis at the molecule/metal oxide interface. As an ideal model for investigating the excitonic effect, coadsorption and photodissociation of water and methanol molecules on titanium dioxide involve complex ground-state thermalcatalytic and excited-state photocatalytic reaction processes. Herein, we systemically investigate the excited-state electronic structures of the coadsorption of H2O and CH3OH molecules on a rutile TiO2(110) surface by linear-response time-dependent density functional theory calculations and probe the reaction path for generating HCOOH or CO2, from ground-state and excited-state perspectives. The reaction barriers in excited-state calculations are significantly different from those in ground-state calculations during three processes, with the largest decrease being 0.94 eV for the Ti5c -O-CH2-O-Ti5c formation process.

SCI ; EI

英语

其他

National Natural Science Foundation of China[XDB0450101] ; Strategic Priority Research Program of the Chinese Academy of Sciences[2021ZD0303306] ; Innovation Program for Quantum Science and Technology["22288201","22173093","21688102"] ; National Natural Science Foundation of China[2022a05020052] ; Anhui Provincial Key Research and Development Program["2016YFA0200604","2021YFB0300600"] ; National Key Research and Development Program of China["CASWX2021SF-0103","KF2020003"]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:001167235300001

AMER CHEMICAL SOC

Web of Science

1.Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China
2.Univ Sci & Technol China, Key Lab Precis & Intelligent Chem, Hefei 230026, Anhui, Peoples R China
3.Hefei Univ Technol, Sch Phys, Hefei 230009, Anhui, Peoples R China
4.Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
5.Univ Sci & Technol China, Hefei Natl Lab, Hefei 230026, Anhui, Peoples R China
6.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
7.Ningbo Univ, Dept Phys, Ningbo 315211, Zhejiang, Peoples R China

Wang, Lei,Liu, Xiaofeng,Wan, Lingyun,et al. Excitonic Effects of the Excited-State Photocatalytic Reaction at the Molecule/Metal Oxide Interface[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2024,15(7).

Wang, Lei.,Liu, Xiaofeng.,Wan, Lingyun.,Gao, Yunzhi.,Wang, Xiaoning.,...&Yang, Jinlong.(2024).Excitonic Effects of the Excited-State Photocatalytic Reaction at the Molecule/Metal Oxide Interface.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,15(7).

Wang, Lei,et al."Excitonic Effects of the Excited-State Photocatalytic Reaction at the Molecule/Metal Oxide Interface".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 15.7(2024).