Intrinsic Role of Excess Electrons in Surface Reactions on Rutile TiO2 (110): Using Water and Oxygen as Probes

Tian, Hao1,2; Xu, Bin3,4; Fan, Jing1; Xu, Hu1

2018-04-19

10.1021/acs.jpcc.7b12451

Journal of Physical Chemistry C   影响因子和分区

1932-7447

Reactions on catalytically active surfaces often involve complex mechanisms with multiple interactions between adsorbates and various subsequently formed intermediates, and a variable number of excess electrons further complicates the involved mechanisms. Experimental techniques face challenges in precisely tuning or determining the number of excess electrons and in elucidating these complex reactions. In this work, the thermodynamic details and reaction pathways of interactions between the most prevalent and important molecular species, H2O and O-2, on a prototypical rutile TiO2 (110) surface are investigated using density functional theory calculations on 10 elementary reaction steps with the intention of gaining further insight into surface catalysis. The results suggest that the final product is independent of the reaction pathway when the number of excess electrons is sufficient. The intrinsic role of excess electrons at the reaction level is thus proposed to extend the understanding of the origin, distribution, and transfer of excess electrons. Such an understanding is beneficial to develop high-performance catalysts.

SCI ; EI

英语

第一 ; 通讯

Basic Research Program of Science, Technology and Innovation Commission of Shenzhen Municipality[JCYJ20160531190054083] ; Basic Research Program of Science, Technology and Innovation Commission of Shenzhen Municipality[JCYJ20170412154426330]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000430896500026

AMER CHEMICAL SOC

20181705051282

Density functional theory ; Electrons ; Oxide minerals ; Oxygen ; Reaction intermediates ; Titanium dioxide

Minerals:482.2 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Probability Theory:922.1

Web of Science

1.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
2.Univ Hong Kong, Dept Phys, Hong Kong, Hong Kong, Peoples R China
3.Univ Arkansas, Phys Dept, Fayetteville, AR 72701 USA
4.Univ Arkansas, Inst Nanosci & Engn, Fayetteville, AR 72701 USA

Tian, Hao,Xu, Bin,Fan, Jing,et al. Intrinsic Role of Excess Electrons in Surface Reactions on Rutile TiO2 (110): Using Water and Oxygen as Probes[J]. Journal of Physical Chemistry C,2018,122(15):8270-8276.

Tian, Hao,Xu, Bin,Fan, Jing,&Xu, Hu.(2018).Intrinsic Role of Excess Electrons in Surface Reactions on Rutile TiO2 (110): Using Water and Oxygen as Probes.Journal of Physical Chemistry C,122(15),8270-8276.

Tian, Hao,et al."Intrinsic Role of Excess Electrons in Surface Reactions on Rutile TiO2 (110): Using Water and Oxygen as Probes".Journal of Physical Chemistry C 122.15(2018):8270-8276.