Heterolytic dissociative adsorption state of dihydrogen favored by interfacial defects

Song, Zhenjun1,2; Hu, Hanshi3,4; Xu, Hu6; Li, Yong5; Cheng, Peng1,2; Zhao, Bin1,2

2018-03

10.1016/j.apsusc.2017.10.124

APPLIED SURFACE SCIENCE   影响因子和分区

0169-4332

1873-5584

The atomic-scale insight into dihydrogen on MgO(001) surface deposited on molybdenum substrate with interfacial defects was investigated in detail by employing density functional methods Here we report novel dissociative adsorption behaviors of single hydrogen molecule on the usually inert oxide surfaces, with consideration of two types of dissociation schemes. The heterolytic dissociation state-Mg(H)-O(H)-of dihydrogen is impossible to obtain on neighboring O-Mg sites of perfect bulk MgO(001) terraces. Unusually, the hydrogen molecule can form heterolytic fragmentation states on metal supported MgO(001) films with very low activation barrier (0.398 eV), and the heterolytic dissociation state is much more favorable than homolytic dissociation state both energetically and kinetically in all cases. Electronic properties and bonding attribution of adsorbates and the oxide-metal hybrid structure are revealed by analyzing density of states, differential charge densities, orbital interaction and electron localization function. The characteristic changes to the property and activity of magnesia (001) can have potential application in catalytic reactions. (C) 2017 Elsevier B.V. All rights reserved.

Heterolytic dissociation Dihydrogen Magnesia Interfacial Defects Density functional theory

SCI ; EI

英语

其他

Project 111[B12015]

Chemistry ; Materials Science ; Physics

Chemistry, Physical ; Materials Science, Coatings & Films ; Physics, Applied ; Physics, Condensed Matter

WOS:000418883800109

ELSEVIER SCIENCE BV

20174304311189

Catalysis ; Chemical bonds ; Defects ; Electronic properties ; Hydrogen ; Magnesia ; Molecules ; Photodissociation ; Surface defects

Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3 ; Materials Science:951

MATERIALS SCIENCE

Web of Science

1.Nankai Univ, Coll Chem, Key Lab Adv Energy Mat Chem, Minist Educ, Tianjin 300071, Peoples R China
2.Nankai Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300071, Peoples R China
3.Tsinghua Univ, Dept Chem, Minist Educ, Beijing 100084, Peoples R China
4.Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China
5.Univ Bremen, Inst Appl & Phys Chem, D-28359 Bremen, Germany
6.South Univ Sci & Technol China, Dept Phys, Shenzhen 518055, Peoples R China

Song, Zhenjun,Hu, Hanshi,Xu, Hu,et al. Heterolytic dissociative adsorption state of dihydrogen favored by interfacial defects[J]. APPLIED SURFACE SCIENCE,2018,433:862-868.

Song, Zhenjun,Hu, Hanshi,Xu, Hu,Li, Yong,Cheng, Peng,&Zhao, Bin.(2018).Heterolytic dissociative adsorption state of dihydrogen favored by interfacial defects.APPLIED SURFACE SCIENCE,433,862-868.

Song, Zhenjun,et al."Heterolytic dissociative adsorption state of dihydrogen favored by interfacial defects".APPLIED SURFACE SCIENCE 433(2018):862-868.