Wavelength-Dependent Water Oxidation on Rutile TiO2 (110)

Xu, Chenbiao1; Xu, Fei2,3; Chen, Xiao4; Li, Zhenxing2,3; Luan, Zhiwen2,3; Wang, Xingan2,3; Guo, Qing4; Yang, Xueming1,4

2021-01-28

10.1021/acs.jpclett.0c03726

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

Understanding the microscopic mechanism of water photocatalysis on TiO2 is of great value in energy chemistry and catalysis. To date, it is still unclear how water photocatalysis occurs after the initial light absorption. Here we report the investigation of the photoinduced water dissociation and desorption on a R-TiO2(110) surface, at different wavelengths (from 250 to 330 nm), using temperature-programmed desorption and time-of-flight techniques. Primary photooxidation products, gas phase OH radicals and surface H atoms, were clearly observed at wavelengths of <= 290 nm. As the laser wavelength decreases from 290 to 250 nm, the relative yield of H2O oxidation increases significantly. Likewise, photoinduced H2O desorption was also observed in the range of 320-250 nm, and the relative yield of H2O desorption also increases with a decrease in wavelength. The strong wavelength-dependent H2O photooxidation and photodesorption suggest that the energy of charge carriers is important in these two processes. More importantly, the result raises doubt about the widely accepted photocatalysis model of TiO2 in which the excess energy of charge carriers is useless for photocatalysis. In addition, the H2O photooxidation is more likely initiated by nonthermalized holes and is accomplished on the ground state potential energy surface via a non-adiabatic decay process.

SCI ; EI

英语

NI期刊 ; NI论文

通讯

National Key R&D Program of China[2018YFE0203002] ; National Natural Science Foundation of China (NSFC Center for Chemical Dynamics)[21673235] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB17000000] ; International Partnership Program of the Chinese Academy of Sciences[121421KYSB20170012] ; Guangdong Innovative & Entrepreneurial Research Team Program["2019ZT08L455","2019JC01X091"] ; Shenzhen Science and Technology Innovation Committee[JCYJ2019080914021660]

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

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

WOS:000614318900015

AMER CHEMICAL SOC

20210509874731

Carrier mobility ; Free radicals ; Ground state ; Light absorption ; Oxide minerals ; Photocatalysis ; Photooxidation ; Potential energy ; Quantum chemistry ; Temperature programmed desorption ; Water absorption

Minerals:482.2 ; Semiconducting Materials:712.1 ; Light/Optics:741.1 ; Physical Chemistry:801.4 ; Chemical Operations:802.3 ; Inorganic Compounds:804.2

Web of Science

1.Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Liaoning, Peoples R China
2.Univ Sci & Technol China, Ctr Adv Chem Phys, Sch Chem & Mat Sci, Hefei 230026, Anhui, Peoples R China
3.Univ Sci & Technol China, Dept Chem Phys, Sch Chem & Mat Sci, Hefei 230026, Anhui, Peoples R China
4.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China

Xu, Chenbiao,Xu, Fei,Chen, Xiao,et al. Wavelength-Dependent Water Oxidation on Rutile TiO2 (110)[J]. Journal of Physical Chemistry Letters,2021,12(3):1066-1072.

Xu, Chenbiao.,Xu, Fei.,Chen, Xiao.,Li, Zhenxing.,Luan, Zhiwen.,...&Yang, Xueming.(2021).Wavelength-Dependent Water Oxidation on Rutile TiO2 (110).Journal of Physical Chemistry Letters,12(3),1066-1072.

Xu, Chenbiao,et al."Wavelength-Dependent Water Oxidation on Rutile TiO2 (110)".Journal of Physical Chemistry Letters 12.3(2021):1066-1072.