Theoretical Investigation of the Reaction Mechanism of the Guaiacol Hydrogenation over a Pt(111) Catalyst

Lu, Jianmin; Behtash, Sina; Mamun, Osman; Heyden, Andreas

doi:10.1021/cs5016244

Theoretical Investigation of the Reaction Mechanism of the Guaiacol Hydrogenation over a Pt(111) Catalyst

Journal Article · Tue Mar 10 00:00:00 UTC 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/cs5016244· OSTI ID:1656912

Lu, Jianmin ^[1]; Behtash, Sina ^[1]; Mamun, Osman ^[1]; Heyden, Andreas ^[1]

University of South Carolina, Columbia, SC (United States)

The reaction mechanism of the mild hydrogenation of guaiacol over Pt(111) has been investigated by density functional theory calculations and microkinetic modeling. Our model suggests that at 573 K, catechol is the preferred reaction product and that any deoxygenation to, for example, phenol or benzene is at least 4 orders of magnitude slower than the production of catechol. Slow deoxygenation of guaiacol can occur by decarbonylation and possibly by hydrogenation of the phenyl ring followed by C–OH bond cleavage. Direct –OH removal without activation of the phenyl ring is found to be at least 5 orders of magnitude slower. Altogether, this study suggests that Pt(111) sites are not active deoxygenation sites and that the experimentally observed deoxygenation activity of Pt catalysts originates likely from the involvement of the catalyst support or Pt step and corner sites.

View Accepted Manuscript (DOE)

Research Organization:: University of South Carolina, Columbia, SC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0007167

OSTI ID:: 1656912

Alternate ID(s):: OSTI ID: 3001217

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 4 Vol. 5; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Theoretical Investigation of the Reaction Mechanism of the Guaiacol Hydrogenation over a Pt(111) Catalyst

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