Ni-Doping Effects on Oxygen Removal from an Orthorhombic Mo2C (001) Surface: A Density Functional Theory Study

Zhou, Mingxia; Cheng, Lei; Choi, Jae-Soon; Liu, Bin; Curtiss, Larry A.; Assary, Rajeev S.

doi:10.1021/acs.jpcc.7b09870

Title: Ni-Doping Effects on Oxygen Removal from an Orthorhombic Mo₂C (001) Surface: A Density Functional Theory Study

Journal Article · Fri Dec 22 00:00:00 EST 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b09870· OSTI ID:1423017

Zhou, Mingxia ^[1]; Cheng, Lei ^[2]; Choi, Jae-Soon ^[3]; Liu, Bin ^[1]; Curtiss, Larry A. ^[2]; Assary, Rajeev S. ^[2]

Kansas State Univ., Manhattan, KS (United States). Dept. of Chemical Engineering
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Density functional theory (DFT) calculations were used to investigate the effect of Ni dopants on the removal of chemisorbed oxygen (O*) from the Mo-terminated (T-Mo) and C-terminated (Tc) Mo2C(001) surfaces. The removal of adsorbed oxygen from the catalytic site is essential to maintain the long-term activity and selectivity of the carbide catalysts in the deoxygenation process related to bio-oil stabilization and upgrading. In this contribution, the computed reaction energetics and reaction barriers of O* removal were compared among undoped and Ni-doped Mo2C(001) surfaces. The DFT calculations indicate that selected Ni-doped surfaces such as Ni adsorbed on T-Mo and Tc Mo2C(001) surfaces enable weaker binding of important reactive intermediates (O*, OH*) compared to the undoped counterparts, which is beneficial for the O* removal from the catalyst surface. This study thus confirms the promoting effect of the Ni dopant on O* removal reaction on the T-Mo Mo2C(001) and Tc Mo2C(001) surfaces. This computational prediction has been confirmed by the temperature-programmed reduction profiles of Mo2C and Ni-doped Mo2C catalysts, which had been passivated and stored in an oxygen environment.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1423017

Alternate ID(s):: OSTI ID: 1425276

Journal Information:: Journal of Physical Chemistry. C, Vol. 122, Issue 3; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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Title: Ni-Doping Effects on Oxygen Removal from an Orthorhombic Mo2C (001) Surface: A Density Functional Theory Study

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