Electrocatalytic Hydrogenation of Furfural with Improved Activity and Selectivity at the Surface of Structured Copper Electrodes
(2024) In ACS Catalysis p.4489-4500- Abstract
Furfural is a pivotal renewable platform molecule obtained from the chemical breakdown of hemicellulose. While it has traditionally been valorized to value-added chemicals through catalytic hydrogenation in biorefineries, its direct electrocatalytic hydrogenation presents attractive advantages. This article describes the significant improvements brought by the structuring of copper cathodes applied to this process in terms of activity and selectivity. We show that structured electrodes are capable of converting furfural to furfuryl alcohol with 100% selectivity at potentials as high as −0.2 V vs the reversible hydrogen electrode (RHE) in neutral conditions (pH 7.0). Moreover, the same electrode can selectively generate either furfuryl... (More)
Furfural is a pivotal renewable platform molecule obtained from the chemical breakdown of hemicellulose. While it has traditionally been valorized to value-added chemicals through catalytic hydrogenation in biorefineries, its direct electrocatalytic hydrogenation presents attractive advantages. This article describes the significant improvements brought by the structuring of copper cathodes applied to this process in terms of activity and selectivity. We show that structured electrodes are capable of converting furfural to furfuryl alcohol with 100% selectivity at potentials as high as −0.2 V vs the reversible hydrogen electrode (RHE) in neutral conditions (pH 7.0). Moreover, the same electrode can selectively generate either furfuryl alcohol or 2-methylfuran in acidic conditions (pH 1.0), depending on the applied potential and temperature. We further show the existence of optimal voltage-temperature conditions for the efficient conversion of furfural to furfuryl alcohol or 2-methylfuran, highlighting the delicate influence of operating conditions on the selectivity of furfural reduction, in competition with the hydrogen evolution reaction in aqueous electrolytes. These performances are attributed to the resilience of Cu(I) species under operating conditions and their likely contribution to the electrocatalytic active site, as revealed by quasi-in situ photoelectron spectroscopy.
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- author
- Spadetto, Clément ; Hachemi, Cyril ; Nouaille-Degorce, Maxime ; Pendu, Loïc ; Bossert, Lou ; Temperton, Robert LU ; Shavorskiy, Andrey LU ; Cardenas, Luis and Prévot, Mathieu S.
- organization
- publishing date
- 2024
- type
- Contribution to journal
- publication status
- epub
- subject
- keywords
- 2-methylfuran, electrocatalytic hydrogenation, furfural, furfuryl alcohol, high-pressure photoemission, in situ, selective
- in
- ACS Catalysis
- pages
- 12 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- scopus:85187579239
- ISSN
- 2155-5435
- DOI
- 10.1021/acscatal.3c05691
- language
- English
- LU publication?
- yes
- id
- 18f731fc-c48f-40c5-aa16-1e525f8260bf
- date added to LUP
- 2024-04-09 13:46:35
- date last changed
- 2024-04-09 13:47:07
@article{18f731fc-c48f-40c5-aa16-1e525f8260bf,
abstract = {{<p>Furfural is a pivotal renewable platform molecule obtained from the chemical breakdown of hemicellulose. While it has traditionally been valorized to value-added chemicals through catalytic hydrogenation in biorefineries, its direct electrocatalytic hydrogenation presents attractive advantages. This article describes the significant improvements brought by the structuring of copper cathodes applied to this process in terms of activity and selectivity. We show that structured electrodes are capable of converting furfural to furfuryl alcohol with 100% selectivity at potentials as high as −0.2 V vs the reversible hydrogen electrode (RHE) in neutral conditions (pH 7.0). Moreover, the same electrode can selectively generate either furfuryl alcohol or 2-methylfuran in acidic conditions (pH 1.0), depending on the applied potential and temperature. We further show the existence of optimal voltage-temperature conditions for the efficient conversion of furfural to furfuryl alcohol or 2-methylfuran, highlighting the delicate influence of operating conditions on the selectivity of furfural reduction, in competition with the hydrogen evolution reaction in aqueous electrolytes. These performances are attributed to the resilience of Cu(I) species under operating conditions and their likely contribution to the electrocatalytic active site, as revealed by quasi-in situ photoelectron spectroscopy.</p>}},
author = {{Spadetto, Clément and Hachemi, Cyril and Nouaille-Degorce, Maxime and Pendu, Loïc and Bossert, Lou and Temperton, Robert and Shavorskiy, Andrey and Cardenas, Luis and Prévot, Mathieu S.}},
issn = {{2155-5435}},
keywords = {{2-methylfuran; electrocatalytic hydrogenation; furfural; furfuryl alcohol; high-pressure photoemission; in situ; selective}},
language = {{eng}},
pages = {{4489--4500}},
publisher = {{The American Chemical Society (ACS)}},
series = {{ACS Catalysis}},
title = {{Electrocatalytic Hydrogenation of Furfural with Improved Activity and Selectivity at the Surface of Structured Copper Electrodes}},
url = {{http://dx.doi.org/10.1021/acscatal.3c05691}},
doi = {{10.1021/acscatal.3c05691}},
year = {{2024}},
}