Tuning the selectivity of biomass oxidation over oxygen evolution on NiO-OH electrodes

Laxman Gouda; Laurent Sévery; Thomas Moehl; Elena Mas-Marzá; Pardis Adams; Francisco Fabregat-Santiago; S. David Tilley

doi:10.1039/d1gc02031e

Tuning the selectivity of biomass oxidation over oxygen evolution on NiO-OH electrodes

Laxman Gouda
, Laurent Sévery
, Thomas Moehl
, Elena Mas-Marzá
, Pardis Adams
, Francisco Fabregat-Santiago
, S. David Tilley

University of Zurich
Jaume I University

Research output: Contribution to journal › Article › peer-review

50 Scopus citations

Abstract

Electrochemical reactions powered by renewable electricity are an important means of reducing the carbon footprint of large-scale chemical processes. Here, we investigate the efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), an important building block in the polymer and pharmaceutical industries, using a cheap and abundant nickel-based electrocatalyst. We elucidate the key factors for tuning the chemical selectivity for HMF oxidation over the competing oxygen evolution reaction (OER) at the catalyst surface. We show that the selectivity for HMF oxidation is enhanced by removing trace impurities of iron species as well as adjusting the composition of the alkali hydroxide electrolyte solution. LiOH solution without iron impurities is more favorable for HMF oxidation, whereas CsOH solution with iron species present is more active for the OER and unfavorable for HMF oxidation. Under optimized conditions, HMF oxidation in 1 M LiOH electrolyte solution without iron (pH 14) achieved 98% faradaic efficiency for the production of FDCA. The principles used in this work can be applied to other electrosynthetic reactions, in particular where the OER is the main competing side reaction.

Original language	English
Pages (from-to)	8061-8068
Number of pages	8
Journal	Green Chemistry
Volume	23
Issue number	20
DOIs	https://doi.org/10.1039/d1gc02031e
State	Published - 21 Oct 2021
Externally published	Yes

Bibliographical note

Publisher Copyright:
© The Royal Society of Chemistry 2021.

Funding

The University of Zurich and the University Research Priority Program (URPP) LightChEC are gratefully acknowledged for funding. The UZH-Center for Microscopy and Image Analysis and Jonas Zurflüh for HPLC analysis are acknowledged for their service. The Institute of Advanced Materials from Universitat Jaume I acknowledges Generalitat Valencia under project- GRISOLIAP/2018/A/070 and Ministerio de Economía y Competitividad (MINECO) under project ENE2017-85087-C3-1-R for financial support. The University of Zurich and the University Research Priority Program (URPP) LightChEC are gratefully acknowledged for funding. The UZH-Center for Microscopy and Image Analysis and Jonas Zurflüh for HPLC analysis are acknowledged for their service. The Institute of Advanced Materials from Universitat Jaume I acknowledges Generalitat Valencia under project-GRISOLIAP/2018/A/070 and Ministerio de Economía y Competitividad (MINECO) under project ENE2017-85087-C3-1-R for financial support.

Funders	Funder number
UZH-Center
Universitat Jaume I acknowledges Generalitat Valencia	project-GRISOLIAP/2018/A/070
Ministerio de Economía y Competitividad	ENE2017-85087-C3-1-R
Universität Zürich

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

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10.1039/d1gc02031e

Cite this

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title = "Tuning the selectivity of biomass oxidation over oxygen evolution on NiO-OH electrodes",

abstract = "Electrochemical reactions powered by renewable electricity are an important means of reducing the carbon footprint of large-scale chemical processes. Here, we investigate the efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), an important building block in the polymer and pharmaceutical industries, using a cheap and abundant nickel-based electrocatalyst. We elucidate the key factors for tuning the chemical selectivity for HMF oxidation over the competing oxygen evolution reaction (OER) at the catalyst surface. We show that the selectivity for HMF oxidation is enhanced by removing trace impurities of iron species as well as adjusting the composition of the alkali hydroxide electrolyte solution. LiOH solution without iron impurities is more favorable for HMF oxidation, whereas CsOH solution with iron species present is more active for the OER and unfavorable for HMF oxidation. Under optimized conditions, HMF oxidation in 1 M LiOH electrolyte solution without iron (pH 14) achieved 98\% faradaic efficiency for the production of FDCA. The principles used in this work can be applied to other electrosynthetic reactions, in particular where the OER is the main competing side reaction.",

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AU - Gouda, Laxman

AU - Sévery, Laurent

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AU - Mas-Marzá, Elena

AU - Adams, Pardis

AU - Fabregat-Santiago, Francisco

AU - Tilley, S. David

PY - 2021/10/21

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N2 - Electrochemical reactions powered by renewable electricity are an important means of reducing the carbon footprint of large-scale chemical processes. Here, we investigate the efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), an important building block in the polymer and pharmaceutical industries, using a cheap and abundant nickel-based electrocatalyst. We elucidate the key factors for tuning the chemical selectivity for HMF oxidation over the competing oxygen evolution reaction (OER) at the catalyst surface. We show that the selectivity for HMF oxidation is enhanced by removing trace impurities of iron species as well as adjusting the composition of the alkali hydroxide electrolyte solution. LiOH solution without iron impurities is more favorable for HMF oxidation, whereas CsOH solution with iron species present is more active for the OER and unfavorable for HMF oxidation. Under optimized conditions, HMF oxidation in 1 M LiOH electrolyte solution without iron (pH 14) achieved 98% faradaic efficiency for the production of FDCA. The principles used in this work can be applied to other electrosynthetic reactions, in particular where the OER is the main competing side reaction.

AB - Electrochemical reactions powered by renewable electricity are an important means of reducing the carbon footprint of large-scale chemical processes. Here, we investigate the efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), an important building block in the polymer and pharmaceutical industries, using a cheap and abundant nickel-based electrocatalyst. We elucidate the key factors for tuning the chemical selectivity for HMF oxidation over the competing oxygen evolution reaction (OER) at the catalyst surface. We show that the selectivity for HMF oxidation is enhanced by removing trace impurities of iron species as well as adjusting the composition of the alkali hydroxide electrolyte solution. LiOH solution without iron impurities is more favorable for HMF oxidation, whereas CsOH solution with iron species present is more active for the OER and unfavorable for HMF oxidation. Under optimized conditions, HMF oxidation in 1 M LiOH electrolyte solution without iron (pH 14) achieved 98% faradaic efficiency for the production of FDCA. The principles used in this work can be applied to other electrosynthetic reactions, in particular where the OER is the main competing side reaction.

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Tuning the selectivity of biomass oxidation over oxygen evolution on NiO-OH electrodes

Abstract

Bibliographical note

Funding

UN SDGs

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