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Carbonate-induced electrosynthesis of hydrogen peroxide via two-electron water oxidation

Carbonate-induced electrosynthesis of hydrogen peroxide via two-electron water oxidation
Carbonate-induced electrosynthesis of hydrogen peroxide via two-electron water oxidation
Electrochemical synthesis of hydrogen peroxide (H2O2), via the two-electron water oxidation reaction (2e– WOR), is an attractive method for the sustainable production of valuable chemicals in place of oxygen during water electrolysis. While the majority of 2e– WOR studies have focussed on electrocatalyst design, little research has been carried out on the selection of the supporting electrolyte. In this work, we investigate the impact of potassium carbonate (K2CO3) electrolytes, and their key properties, on H2O2 production. We find that at electrolyte pH values (> 9.5) where the carbonate anion (CO32–) is prevalent in the mixture, a 26.5% increase in the Faraday efficiency (%FE) for H2O2 production is achieved, compared to bicarbonate (HCO3–) dominant solutions. Utilising boron-doped diamond (BDD) in highly concentrated K2CO3 solutions, current densities of up to 511 mA cm-2 (in 4 M) and %FEs of 91.5% (in 5 M) can be attained. The results presented in this work highlight the influence of CO32– on electrochemical H2O2 generation via the 2e– WOR and provide novel pathways to produce desirable commodities at the anode during electrochemical water splitting.
boron-doped diamond (BDD);, carbonate (CO32–);, electrochemistry;, electrolyte;, hydrogen peroxide (H2O2);, oxidation, two-electron water oxidation reaction (2e– WOR);, water chemistry
1864-5631
Mavrikis, Sotirios
6b5b53fb-a664-4c2e-b17d-5c27850d6ea9
Goltz, Maximilian
d12adaf6-5a36-4980-b19d-e0d7684fcc66
Rosiwal, Stefan
a9289623-ffd3-4975-ac52-aa258f19c1f4
Wang, Ling
c50767b1-7474-4094-9b06-4fe64e9fe362
Ponce De Leon Albarran, Carlos
508a312e-75ff-4bcb-9151-dacc424d755c
Mavrikis, Sotirios
6b5b53fb-a664-4c2e-b17d-5c27850d6ea9
Goltz, Maximilian
d12adaf6-5a36-4980-b19d-e0d7684fcc66
Rosiwal, Stefan
a9289623-ffd3-4975-ac52-aa258f19c1f4
Wang, Ling
c50767b1-7474-4094-9b06-4fe64e9fe362
Ponce De Leon Albarran, Carlos
508a312e-75ff-4bcb-9151-dacc424d755c

Mavrikis, Sotirios, Goltz, Maximilian, Rosiwal, Stefan, Wang, Ling and Ponce De Leon Albarran, Carlos (2021) Carbonate-induced electrosynthesis of hydrogen peroxide via two-electron water oxidation. ChemSusChem. (doi:10.1002/cssc.202102137).

Record type: Article

Abstract

Electrochemical synthesis of hydrogen peroxide (H2O2), via the two-electron water oxidation reaction (2e– WOR), is an attractive method for the sustainable production of valuable chemicals in place of oxygen during water electrolysis. While the majority of 2e– WOR studies have focussed on electrocatalyst design, little research has been carried out on the selection of the supporting electrolyte. In this work, we investigate the impact of potassium carbonate (K2CO3) electrolytes, and their key properties, on H2O2 production. We find that at electrolyte pH values (> 9.5) where the carbonate anion (CO32–) is prevalent in the mixture, a 26.5% increase in the Faraday efficiency (%FE) for H2O2 production is achieved, compared to bicarbonate (HCO3–) dominant solutions. Utilising boron-doped diamond (BDD) in highly concentrated K2CO3 solutions, current densities of up to 511 mA cm-2 (in 4 M) and %FEs of 91.5% (in 5 M) can be attained. The results presented in this work highlight the influence of CO32– on electrochemical H2O2 generation via the 2e– WOR and provide novel pathways to produce desirable commodities at the anode during electrochemical water splitting.

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Accepted/In Press date: 21 December 2021
e-pub ahead of print date: 21 December 2021
Keywords: boron-doped diamond (BDD);, carbonate (CO32–);, electrochemistry;, electrolyte;, hydrogen peroxide (H2O2);, oxidation, two-electron water oxidation reaction (2e– WOR);, water chemistry

Identifiers

Local EPrints ID: 454109
URI: http://eprints.soton.ac.uk/id/eprint/454109
ISSN: 1864-5631
PURE UUID: 3873a4b0-ade6-46d7-9a72-cba94cf86a59
ORCID for Ling Wang: ORCID iD orcid.org/0000-0002-2894-6784
ORCID for Carlos Ponce De Leon Albarran: ORCID iD orcid.org/0000-0002-1907-5913

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Date deposited: 31 Jan 2022 17:41
Last modified: 17 Mar 2024 07:02

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Contributors

Author: Sotirios Mavrikis
Author: Maximilian Goltz
Author: Stefan Rosiwal
Author: Ling Wang ORCID iD

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