Hydrothermally stable, conformal, sulfated zirconia monolayer catalysts for glucose conversion to 5-HMF


The grafting and sulfation of zirconia conformal monolayers on SBA-15 to create mesoporous catalysts of tunable solid acid/base character is reported. Conformal zirconia and sulfated zirconia (SZ) materials exhibit both Brönsted and Lewis acidity, with the Brönsted/Lewis acid ratio increasing with film thickness and sulfate content. Grafted zirconia films also exhibit amphoteric character, whose Brönsted/Lewis acid site ratio increases with sulfate loading at the expense of base sites. Bilayer ZrO2/SBA-15 affords an ordered mesoporous material with a high acid site loading upon sulfation and excellent hydrothermal stability. Catalytic performance of SZ/SBA-15 was explored in the aqueous phase conversion of glucose to 5-HMF, delivering a 3-fold enhancement in 5-HMF productivity over nonporous SZ counterparts. The coexistence of accessible solid basic/Lewis acid and Brönsted acid sites in grafted SZ/SBA-15 promotes the respective isomerization of glucose to fructose and dehydration of reactively formed fructose to the desired 5-HMF platform chemical.

Publication DOI: https://doi.org/10.1021/acscatal.5b00965
Divisions: College of Engineering & Physical Sciences
College of Engineering & Physical Sciences > School of Infrastructure and Sustainable Engineering > Chemical Engineering & Applied Chemistry
College of Engineering & Physical Sciences > Energy and Bioproducts Research Institute (EBRI)
Additional Information: This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. Funding: European Union Seventh Framework Programme (FP7/2007-2013) Grant Agreement No. 604307; EPSRC (EP/K014676/1; EP/G007594/4); Royal Society (IF100206); Ministerio de Ciencia e Innovación of Spain (CTQ2011-28216); and Regional Government of Madrid (S2013-MAE-288) Supporting information avaialble online.
Uncontrolled Keywords: SBA-15,solid base,hydrothermal stability,5-HMF,solid acid,sulfated zirconia,Catalysis
Publication ISSN: 2155-5435
Last Modified: 18 Jun 2024 07:13
Date Deposited: 12 Oct 2015 11:10
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Related URLs: http://www.scop ... tnerID=8YFLogxK (Scopus URL)
PURE Output Type: Article
Published Date: 2015-06-17
Authors: Osatiashtiani, Amin (ORCID Profile 0000-0003-1334-127X)
Lee, Adam F. (ORCID Profile 0000-0002-2153-1391)
Granollers, Marta (ORCID Profile 0000-0001-8602-9362)
Brown, D. Robert
Olivi, Luca
Morales, Gabriel
Melero, Juan A.
Wilson, Karen (ORCID Profile 0000-0003-4873-708X)



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