Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 243, Issue -, Pages 337-354Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2018.10.036
Keywords
2,5-Dimethylfuran; Disaccharide; Direct conversion; Tandem catalyst; UiO-66(NH2)
Funding
- National Research Foundation of Korea (NRF) grant - Korean Government (MSIP) [2016R1D1A1B039340602016R1A2B3008800, 2015H1D3A1066544, 2016R1D1A1B03934060]
- Technology Development Program to Solve Climate Changes of the National Research Foundation (NRF) - Ministry of Science, ICT AMP
- Future Planning [2017M1A2A2087635]
- National Research Foundation of Korea [2015H1D3A1066544, 2017M1A2A2087635, 2016R1D1A1B03934060] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Tandem heterogenous catalysis of bimetallic Cu-Pd on UiO-66(NH2) that were incorporated into sulfonated graphene oxide (Cu-Pd/UiO-66(NH2)@SGO or Cu-Pd/US) was investigated for the one-pot, direct conversion of di- and polysaccharides into 2,5-dimethylfuran (2,5-DMF) without separation of reaction intermediates. In the absence of a homogeneous acidic catalyst, consecutive reactions of glycosidic bond cleavage, isomerization, dehydration, and hydrogenation/hydrogenolysis were preceded by the synergistic effect of a multifunctional Cu-Pd/US catalyst. The strength and ratio of Bronsted and Lewis acid sites by adjusting UiO-66(NH2) to SGO ratios resulted in high-yield 5-(hydroxymethyl)furfural (5-HMF) through sequential glycosidic bond cleavage, isomerization, and dehydration of sucrose. Unlike monometallic Cu and Pd, bimetallic Cu-Pd promoted consecutive C-OH hydrogenolysis and C=O hydrogenation of reaction intermediates, producing 2,5-DMF with a high yield of 73.4% during the one-pot conversion of sucrose at 200 degrees C and 1 MPa H-2 for 3 h. When starch was converted over Cu-Pd/US, 2,5-DMF was formed with 53.6% yield. Direct cellulose conversion into 2,5-DMF with a yield of 29.8% was achieved in the presence of 0.01 M HCl and Cu-Pd/US. The presence of the amino functional group (-NH2) in the UiO-66 framework was beneficial for improving the feed conversion and maintaining catalyst recyclability up to five times with almost no activity loss.
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