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J Am Chem Soc

Title:		Photooxidation of Isoprene by Titanium Oxide Cluster Anions with Dimensions up to a Nanosize
Author(s):		Lv SY; Liu QY; Zhao YX; He SG;
Address:		"State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China. University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China. Beijing National Laboratory for Molecular Sciences and CAS Research/Education Center of Excellence in Molecular Sciences, Beijing 100190, People's Republic of China"
Journal Title:		J Am Chem Soc
Year:		2021
Volume:		20210303
Issue:		10
Page Number:		3951 - 3958
DOI:		10.1021/jacs.1c00326
ISSN/ISBN:		1520-5126 (Electronic) 0002-7863 (Linking)
Abstract:		"Titania (TiO(2)) nanoparticles are active photocatalysts, and isoprene (C(5)H(8)) is a biogenic volatile organic compound that contributes crucially to global particulate matter generation. Herein, the direct photooxidation of isoprene by titanium oxide cluster anions with dimensions up to a nanosize by both ultraviolet (UV) and visible (Vis) light excitations has been successfully identified through mass spectrometric experiments combined with quantum chemistry calculations. The potential role of 'dry' titania in atmospheric isoprene oxidation has been revealed, and a clear picture of the photooxidation mechanism on titanium oxide nanoparticles has been provided explicitly at the molecular level. The adsorption of isoprene on the atomic oxygen radicals (O(*-)) of titanium oxide clusters leads to the formation of the crucial interfacial state (IS) within the band gap of titanium oxides. This IS is demonstrated to be the significant factor in delivering the electron from the pi orbital of C(5)H(8) to the Ti(3d) orbital in the photooxidation process (C(5)H(8) + Ti(4)(+)-O(*-) --> C(5)H(8)O + Ti(3)(+)) and creating photoactivity in the Vis region. It is revealed that after the photogeneration of the O(*-) radicals by UV excitation on the TiO(2) particle surface, the subsequent reactions can be induced by Vis excitation through the IS. This multicolor strategy in both the UV and Vis regions can enhance the efficiency of solar energy harvesting and improve the product yield of the photocatalysis on TiO(2) nanoparticles. New insights have been provided into both the atmospheric chemistry of isoprene and the photochemistry of TiO(2) nanoparticles"
Keywords:
Notes:		"PubMed-not-MEDLINELv, Shi-Ying Liu, Qing-Yu Zhao, Yan-Xia He, Sheng-Gui eng 2021/03/04 J Am Chem Soc. 2021 Mar 17; 143(10):3951-3958. doi: 10.1021/jacs.1c00326. Epub 2021 Mar 3"