Activation of CO2 by Direct Cleavage Triggered by Photoelectrons on Rutile TiO2(110)

Zhao，Changming; Xu，Hu

2023-02-23

10.1021/acs.jpclett.3c00040

Journal of Physical Chemistry Letters   Impact Factor & Quartile

1948-7185

1948-7185

The initial activation of the inert CO is a key step in its photoreduction to valuable chemicals. This process was proposed to proceed mainly by CO accepting a photoelectron to form a CO radical or by CO accepting two photoelectrons and a proton to form the HCOO anion on the prototypical rutile TiO(110) surface. Here, we reveal a new mechanism, in which CO is directly cleaved to CO and the adsorbed O anion under the trigger of two photoelectrons, by using density functional theory calculations with the HSE06 hybrid functional. The newly revealed mechanism is more favorable than the two previously proposed pathways. Furthermore, our results show that the deficiency of photoelectrons on the catalyst surface is a potential reason for the current low efficiency of CO photoreduction.

SCI

English

NI Journal Papers

First ; Corresponding

Science, Technology, and Innovation Commission of Shenzhen Municipality[RCYX20200714114523069] ; National Natural Science Foundation of China[11974160]

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

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

WOS:000937469900001

AMER CHEMICAL SOC

2-s2.0-85148340548

Scopus

Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China

Zhao，Changming,Xu，Hu. Activation of CO2 by Direct Cleavage Triggered by Photoelectrons on Rutile TiO2(110)[J]. Journal of Physical Chemistry Letters,2023,14(7):1928-1933.

Zhao，Changming,&Xu，Hu.(2023).Activation of CO2 by Direct Cleavage Triggered by Photoelectrons on Rutile TiO2(110).Journal of Physical Chemistry Letters,14(7),1928-1933.

Zhao，Changming,et al."Activation of CO2 by Direct Cleavage Triggered by Photoelectrons on Rutile TiO2(110)".Journal of Physical Chemistry Letters 14.7(2023):1928-1933.