Effect of hydrogen coverage on hydrogenation of o-cresol on Pt(111)

Li, Yaping; Liu, Zhimin; Crossley, Steven P.; Jentoft, Friederike C.; Wang, Sanwu

doi:10.1016/j.apsusc.2018.02.288

Title: Effect of hydrogen coverage on hydrogenation of o-cresol on Pt(111)

Journal Article · 02 March 2018 · Applied Surface Science

DOI: https://doi.org/10.1016/j.apsusc.2018.02.288 · OSTI ID:1462043

Li, Yaping ^[1]; Liu, Zhimin ^[2]; Crossley, Steven P. ^[2]; Jentoft, Friederike C. ^[3]; Wang, Sanwu ^[1]

Univ. of Tulsa, Tulsa, OK (United States)
Univ. of Oklahoma, Norman, OK (United States)
Univ. of Oklahoma, Norman, OK (United States); Univ. of Massachusetts, Amherst, MA (United States)

The conversion of phenolics over metal catalysts is an important process for upgrading biofuels. With density functional calculations, hydrogenation of o-cresol on the hydrogen-covered Pt(111) surface was investigated. Here, the results show that the coverage of hydrogen plays a significant role in the reaction rate while it does not affect the reaction selectivity. The reaction barriers of the hydrogenation process leading to the formation of both 2-methyl-cyclohexanone (the intermediate product) and 2-methyl-cyclohexanol (the final product) at high H coverages (~ 1 ML) are found to be smaller by 0.14–0.69 eV than those at lower H coverages (~ 1/25 ML). After both hydrogen and cresol are adsorbed on Pt(111) from their initial gas phase state, the reaction energy of each hydrogenation step on the surface is also dependent on the hydrogen coverage. On the H-covered Pt(111) surface, most steps of hydrogenation involve exothermic reactions when the hydrogen coverage is high while they are endothermic reactions at low hydrogen coverages. The differences in reaction rate and reaction energy between high and low H coverages can be understood with the coverage-dependent bonding strength and configurations.

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Research Organization:: Lawrence Berkeley National Laboratory, Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR); USDOE

Grant/Contract Number:: AC02-05CH11231; SC0004600

OSTI ID:: 1462043

Alternate ID(s):: OSTI ID: 1582971

Journal Information:: Applied Surface Science, Vol. 443, Issue C; ISSN 0169-4332

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 10 works

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08 HYDROGEN
Hydrogenation
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Platinum catalyst
Ab initio calculations
Hydrogen coverages
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Title: Effect of hydrogen coverage on hydrogenation of o-cresol on Pt(111)

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