Mechanistic Study of the Direct Hydrodeoxygenation of m-Cresol over WOx-Decorated Pt/C Catalysts

Wang, Cong; Mironenko, Alexander V.; Raizada, Abhishek; Chen, Tianqi; Mao, Xinyu; Padmanabhan, Ashwin; Vlachos, Dionisios G.; Gorte, Raymond J.; Vohs, John M.

doi:10.1021/acscatal.8b01746

Mechanistic Study of the Direct Hydrodeoxygenation of m-Cresol over WO_x-Decorated Pt/C Catalysts

Journal Article · Fri Jul 13 00:00:00 EDT 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b01746· OSTI ID:1539510

^[1]; Mironenko, Alexander V. ^[2]; Raizada, Abhishek ^[3]; Chen, Tianqi ^[3]; Mao, Xinyu ^[3]; Padmanabhan, Ashwin ^[3]; ^[2]; Gorte, Raymond J. ^[4]; ^[3]

University of Pennsylvania, Philadelphia, PA (United States); University of Delaware, Newark, DE (United States); DOE/OSTI
University of Delaware, Newark, DE (United States)
University of Pennsylvania, Philadelphia, PA (United States)
University of Pennsylvania, Philadelphia, PA (United States); University of Delaware, Newark, DE (United States)

In this report hydrodeoxygenation (HDO) of m-cresol to produce toluene over carbon-supported Pt and Pt-WOx catalysts was studied. In stark contrast to Pt/C that exhibits only modest selectivity and low stability for this reaction, Pt-WOx/C was found to be unusually active and selective to toluene with greater than 94% selectivity to this product while exhibiting little to no deactivation under a wide range of reaction conditions. Reactivity studies in combination with density functional theory (DFT) calculations for the adsorption and reaction of m-cresol on structurally optimized WOx-decorated Pt(111) structures indicate that the HDO reaction on Pt-WOx/C proceeds via a direct hydrogenolysis of the C–O bond in m-cresol adsorbed on oxygen vacancy (or redox) sites on WOx species. The DFT results also indicate that Pt helps stabilize the WOx film while facilitating oxygen vacancy formation.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States); University of Delaware, Newark, DE (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0001004

OSTI ID:: 1539510

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 9 Vol. 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Pt-WOx/C catalyst
density functional theory
hydrodeoxygenation
lignin
m-cresol
toluene

Mechanistic Study of the Direct Hydrodeoxygenation of m-Cresol over WOx-Decorated Pt/C Catalysts

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