Title: Efficient dual acidic carbo-catalyst for one-pot conversion of carbohydrates to levulinic acid

Abstract

Levulinic acid (LA) is an important platform intermediate for several high value renewable bioproducts. One-pot synthesis of LA from carbohydrates is disadvantaged by the lack of proximity of the active sites required for sequential isomerization, dehydration and rehydration reactions. Herein, we report an efficient one-pot conversion of C ₆ sugars to LA using a carbo-catalyst (ZrHyC), containing Lewis acidic zirconium and Brønsted acidic carboxyl and hydroxyl sites. The proximity of the two acid sites on a hydrothermally prepared carbon support makes the catalyst highly effective enabling a maximum 73% LA yield from glucose conversion. Fructose conversion achieved a higher LA yield (89%) because of a facile reaction without involving an isomerization step. The effects of solvents, the glucose to catalyst ratio, and the reaction time on glucose conversion and LA yield are systemically examined. Detailed characterization of the catalyst using FTIR, Raman spectroscopy, XPS, XRD, FESEM and NH ₃-TPD techniques are presented to elucidate the presence of the two acid sites and zirconium in the +4 oxidation state.

Authors:

Gupta, Dinesh ^[1]; Kundu, Sabuj ^[2]; Saha, Basudeb ^[3]

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+ Show Author Affiliations

1. Univ. of Delhi, New Delhi (India). Lab. of Catalysis, Dept. of Chemistry; Indian Inst. of Technology Kanpur, Kanpur (India). Dept. of Chemistry
2. Indian Inst. of Technology Kanpur, Kanpur (India). Dept. of Chemistry
3. Univ. of Delhi, New Delhi (India). Lab. of Catalysis, Dept. of Chemistry; Univ. of Delaware, Newark, DE (United States). Catalysis Center for Energy Innovation

Publication Date:

2016-10-21

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)

Sponsoring Org.:

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

OSTI Identifier:

1388587

Grant/Contract Number:  

SC0001004

Resource Type:

Journal Article: Accepted Manuscript

Journal Name:

RSC Advances

Additional Journal Information:

Journal Volume: 6; Journal Issue: 102; Related Information: CCEI partners with the University of Delaware (lead); Brookhaven National Laboratory; California Institute of Technology; Columbia University; University of Delaware; Lehigh University; University of Massachusetts, Amherst; Massachusetts Institute of Technology; University of Minnesota; Pacific Northwest National Laboratory; University of Pennsylvania; Princeton University; Rutgers University; Journal ID: ISSN 2046-2069

Publisher:

Royal Society of Chemistry

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 09 BIOMASS FUELS; catalysis (homogeneous); catalysis (heterogeneous); biofuels (including algae and biomass); bio-inspired; hydrogen and fuel cells; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)