Interaction of Atomic Deuterium with Rutile TiO2(011)-(2×1)

Chen，Wei1,4; Gao，Yajie1,4; Wang，Tianjun1; Hao，Qunqing1; Wang，Zhiqiang2; Ren，Zefeng1; Yang，Xueming1,3; Zhou，Chuanyao1,4

2023

10.1021/acs.jpcc.3c00815

Journal of Physical Chemistry C   影响因子和分区

1932-7447

1932-7455

Inspired by the significance of hydrogen-solid interaction in hydrogen energy and catalysis, adsorption, diffusion, and desorption behaviors of deuterium atoms in rutile TiO(011) have been investigated by temperature-programmed desorption (TPD) and ultraviolet photoelectron spectroscopy (UPS). Upon exposure, a small portion of D atoms adsorb at surface oxygen sites, resulting in the band gap states at 1.35 eV below the Fermi level and desorbing as water at ∼400 K. Most of the D atoms will diffuse into the bulk due to the relatively low activation barrier and the huge capacity of the solid material. These bulk D species desorb as D/HD between 500 and 800 K. While the desorbing DO from surface hydroxyls saturates at ∼0.10 monolayer (ML), the yielding D is about 96 ML (equivalent coverage) at the largest atomic D exposure of 4.54 langmuir and no saturation trend has been observed in the present work. Detailed analysis indicates the bulk D will diffuse back to the surface and recombine as D at elevated temperatures. The differences between the behavior of H(D) in rutile TiO(110) and TiO(011) have been discussed by considering the presence of additional bridging oxygen atoms between the in-plane and topmost ones on the latter surface. The striking finding that most surface D atoms diffuse into the bulk of rutile TiO(011) will not only broaden our understanding of the interaction of H/D with the prototypical metal oxide material but also provide clues to investigate the mechanism of H/D involving reactions over TiO catalysts, for example, hydrogen evolution and hydrogenation.

SCI ; EI

英语

其他

WOS:000966818400001

20231413846673

Atoms ; Deuterium ; Energy gap ; Monolayers ; Oxide minerals ; Oxygen ; Photoelectron spectroscopy ; Temperature programmed desorption

Minerals:482.2 ; Chemical Operations:802.3 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

2-s2.0-85151388115

Scopus

1.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,457 Zhongshan Road, Liaoning,116023,China
2.School of Physics,Xidian University,Xi’an,Shaanxi,710071,China
3.Department of Chemistry,Southern University of Science and Technology,Shenzhen,1088 Xueyuan Road, Guangdong,518055,China
4.University of Chinese Academy of Sciences,Beijing,No. 19A Yuquan Road,100049,China

Chen，Wei,Gao，Yajie,Wang，Tianjun,et al. Interaction of Atomic Deuterium with Rutile TiO2(011)-(2×1)[J]. Journal of Physical Chemistry C,2023,127:6723-6732.

Chen，Wei.,Gao，Yajie.,Wang，Tianjun.,Hao，Qunqing.,Wang，Zhiqiang.,...&Zhou，Chuanyao.(2023).Interaction of Atomic Deuterium with Rutile TiO2(011)-(2×1).Journal of Physical Chemistry C,127,6723-6732.

Chen，Wei,et al."Interaction of Atomic Deuterium with Rutile TiO2(011)-(2×1)".Journal of Physical Chemistry C 127(2023):6723-6732.