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Photoelectrochemical oxidation in ambient conditions using earth-abundant hematite anode : A green route for the synthesis of biobased polymer building blocks

Kawde, Anurag LU ; Sayed, Mahmoud LU orcid ; Shi, Qi LU ; Uhlig, Jens LU ; Pullerits, Tönu LU and Hatti-Kaul, Rajni LU (2021) In Catalysts 11(8).
Abstract

This study demonstrates the use of a photoelectrochemical device comprising earth-abundant hematite photoanode for the oxidation of 5-hydroxymethylfurfural (5-HMF), a versatile bio-based platform chemical, under ambient conditions in the presence of an electron mediator. The results obtained in this study showed that the hematite photoanode, upon doping with fluorine, can oxidize water even at lower pH (4.5 and 9.0). For 5-HMF oxidation, three different pH conditions were investigated, and complete oxidation to 2,5-furandicarboxylic acid (FDCA) via 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) was achieved at pH above 12. At lower pH, the oxidation followed another route via 2,5-diformylfuran (DFF), yielding 5-formyl-2-furancarboxylic... (More)

This study demonstrates the use of a photoelectrochemical device comprising earth-abundant hematite photoanode for the oxidation of 5-hydroxymethylfurfural (5-HMF), a versatile bio-based platform chemical, under ambient conditions in the presence of an electron mediator. The results obtained in this study showed that the hematite photoanode, upon doping with fluorine, can oxidize water even at lower pH (4.5 and 9.0). For 5-HMF oxidation, three different pH conditions were investigated, and complete oxidation to 2,5-furandicarboxylic acid (FDCA) via 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) was achieved at pH above 12. At lower pH, the oxidation followed another route via 2,5-diformylfuran (DFF), yielding 5-formyl-2-furancarboxylic acid (FFCA) as the main product. Using the oxidized intermediates as substrates showed DFF to be most efficiently oxidized to FDCA. We also show that, at pH 4.5, the addition of the laccase enzyme promoted the oxidation of 5-HMF to FFCA.

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
2,5-furandicarboxylic acid, 5-HMF oxidation, Bio-based chemicals, Earth-abundant hematite photoanode, Photoelectrochemical cell
in
Catalysts
volume
11
issue
8
article number
969
pages
12 pages
publisher
MDPI AG
external identifiers
  • scopus:85112364822
ISSN
2073-4344
DOI
10.3390/catal11080969
project
STEPS – Sustainable Plastics and Transition Pathways, Phase 2
language
English
LU publication?
yes
id
b4244eaa-bf7f-49ae-a96a-dabe4683037d
date added to LUP
2021-09-08 10:13:42
date last changed
2024-08-10 20:43:21
@article{b4244eaa-bf7f-49ae-a96a-dabe4683037d,
  abstract     = {{<p>This study demonstrates the use of a photoelectrochemical device comprising earth-abundant hematite photoanode for the oxidation of 5-hydroxymethylfurfural (5-HMF), a versatile bio-based platform chemical, under ambient conditions in the presence of an electron mediator. The results obtained in this study showed that the hematite photoanode, upon doping with fluorine, can oxidize water even at lower pH (4.5 and 9.0). For 5-HMF oxidation, three different pH conditions were investigated, and complete oxidation to 2,5-furandicarboxylic acid (FDCA) via 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) was achieved at pH above 12. At lower pH, the oxidation followed another route via 2,5-diformylfuran (DFF), yielding 5-formyl-2-furancarboxylic acid (FFCA) as the main product. Using the oxidized intermediates as substrates showed DFF to be most efficiently oxidized to FDCA. We also show that, at pH 4.5, the addition of the laccase enzyme promoted the oxidation of 5-HMF to FFCA.</p>}},
  author       = {{Kawde, Anurag and Sayed, Mahmoud and Shi, Qi and Uhlig, Jens and Pullerits, Tönu and Hatti-Kaul, Rajni}},
  issn         = {{2073-4344}},
  keywords     = {{2,5-furandicarboxylic acid; 5-HMF oxidation; Bio-based chemicals; Earth-abundant hematite photoanode; Photoelectrochemical cell}},
  language     = {{eng}},
  number       = {{8}},
  publisher    = {{MDPI AG}},
  series       = {{Catalysts}},
  title        = {{Photoelectrochemical oxidation in ambient conditions using earth-abundant hematite anode : A green route for the synthesis of biobased polymer building blocks}},
  url          = {{http://dx.doi.org/10.3390/catal11080969}},
  doi          = {{10.3390/catal11080969}},
  volume       = {{11}},
  year         = {{2021}},
}