Mechanistic study of the ceria supported, re-catalyzed deoxydehydration of vicinal OH groups

Xi, Yongjie; Yang, Wenqiang; Ammal, Salai Cheettu; Lauterbach, Jochen; Pagan-Torres, Yomaira; Heyden, Andreas

doi:10.1039/c8cy01782d

Title: Mechanistic study of the ceria supported, re-catalyzed deoxydehydration of vicinal OH groups

Journal Article · Mon Jan 01 00:00:00 EST 2018 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/c8cy01782d· OSTI ID:1543806

Xi, Yongjie ^[1]; Yang, Wenqiang ^[1]; Ammal, Salai Cheettu ^[1]; Lauterbach, Jochen ^[1]; Pagan-Torres, Yomaira ^[2];

^[1]

Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
Univ. of Puerto Rico-Mayaguez Campus; Mayaguez (Puerto Rico). Dept. of Chemical Engineering

Deoxydehydration (DODH) is an emerging biomass deoxygenation process whereby vicinal OH groups are removed. Based on DFT calculations and microkinetic modeling, we seek to understand the mechanism of the Re-catalyzed deoxydehydration supported on CeO₂(111). In addition, we aim at understanding the promotional effect of Pd in a heterogeneous ReO_x–Pd/CeO₂ DODH catalyst system. We disentangle the contribution of the oxide support, the oxide-supported single ReO_x species, and a co-adsorbed Pd promoter that has no direct interaction with the Re species. In the absence of a nearby Pd cluster, a Re site is able to reduce subsurface Ce-ions of a hydroxylated CeO₂(111) surface, leading to a catalytically active Re +6 species. The effect of Pd is twofold: (i) Pd catalyzes the hydrogen dissociation and spillover onto CeO₂, which is an indispensable process for the regeneration of the Re catalyst, and (ii) Pd adsorbed in close proximity to Re on CeO2(111) facilitates the oxidation of Re to a +7 oxidation state, which leads to an even more active Re species than the Re +6 site present in the absence of Pd. The latter promotional effect of Pd (and change in oxidation state of Re) disappears with increasing Pd–Re distance and in the presence of oxygen defects on the ceria support. Under these conditions, the ReO_x–Pd/CeO₂ catalyst system exhibits appreciable activity consistent with recent experiments. The established mechanism and role of various species in the catalyst system help to better understand the deoxydehydration catalysis. Also, the importance of the Re oxidation state and the identified oxidation state modification mechanisms suggest a new pathway for tuning the properties of metal-oxide supported catalysts.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1543806

Journal Information:: Catalysis Science and Technology, Vol. 8, Issue 22; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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