Generation of molybdenum hydride species via addition of molecular hydrogen across metal-oxygen bond at monolayer oxide/metal composite interface

Song，Zhenjun1,2; Shao，Xiji3,4; Wang，Qiang5; Ma，Chunxin6; Wang，Kedong3; Han，Deman1

2020-01-24

10.1016/j.ijhydene.2019.11.135

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY   影响因子和分区

0360-3199

1879-3487

Generation of molybdenum hydride species on monolayer oxide/metal composite via addition of molecular hydrogen across metal-oxygen bond is investigated for the first time utilizing periodic Van der Waals density-functional calculations. Lewis acid-base pair constructed by the interfacially defected oxide film and the metal support provides novel active sites for activating H. The produced heterolytic dissociative state exhibits negative dissociative adsorption energy of −0.315 eV which thermodynamically facilitate the dissociation process of H on insulating oxide films. The penitential energy pathways are calculated to reveal the dynamics and reaction processes for H splitting at the oxide-metal interface. The differential charge density contour, electronic density plots, particular occupied orbitals, work function and electron localization function of H dissociation are interpreted to better understand the electronic properties of the unique dissociation behavior of H at interfacially defected magnesia. It is anticipated that the results here could help understand the mechanism of hydrogenation reactions on nanostructured oxide film and provide useful clue for enhancing the reactivity of insulating oxide toward activating H.

Electronic properties Hydrogenation Molybdenum hydride Oxide-metal composite Potential energy profile Thermodynamics

SCI ; EI

英语

其他

Taizhou Municipal Science and Technology Bureau[] ; Beijing Science and Technology Planning Project[1901GY21] ; National Natural Science Foundation of China[21375092] ; National Natural Science Foundation of China[] ; [2018PY023]

Chemistry ; Electrochemistry ; Energy & Fuels

Chemistry, Physical ; Electrochemistry ; Energy & Fuels

WOS:000513294900046

Elsevier Ltd

20195007829618

Chemical activation ; Defects ; Electronic properties ; Hydrides ; Hydrogen ; Hydrogenation ; Magnesia ; Metals ; Molecular oxygen ; Molecular physics ; Molybdenum oxide ; Monolayers ; Photodissociation ; Potential energy ; Thermodynamics ; Van der Waals forces

Thermodynamics:641.1 ; 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

ENGINEERING

2-s2.0-85076237737

Scopus

1.School of Pharmaceutical and Materials Engineering,Taizhou University,Taizhou,318000,China
2.Department of Chemistry,Key Laboratory of Advanced Energy Material Chemistry (MOE),Nankai University,Tianjin,300071,China
3.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China
4.Harbin Institute of Technology,Harbin,150080,China
5.State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan,030001,China
6.State Key Laboratory of Marine Resources Utilization in South China Sea,Hainan University,Haikou,570228,China

Song，Zhenjun,Shao，Xiji,Wang，Qiang,et al. Generation of molybdenum hydride species via addition of molecular hydrogen across metal-oxygen bond at monolayer oxide/metal composite interface[J]. INTERNATIONAL JOURNAL OF HYDROGEN ENERGY,2020,45(4):2975-2988.

Song，Zhenjun,Shao，Xiji,Wang，Qiang,Ma，Chunxin,Wang，Kedong,&Han，Deman.(2020).Generation of molybdenum hydride species via addition of molecular hydrogen across metal-oxygen bond at monolayer oxide/metal composite interface.INTERNATIONAL JOURNAL OF HYDROGEN ENERGY,45(4),2975-2988.

Song，Zhenjun,et al."Generation of molybdenum hydride species via addition of molecular hydrogen across metal-oxygen bond at monolayer oxide/metal composite interface".INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 45.4(2020):2975-2988.