Electrochemical – chemical cycle for high-efficiency decoupled water splitting in a near-neutral electrolyte

20 October 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Green hydrogen produced by water splitting using renewable electricity is essential to achieve net-zero carbon emissions. Present water electrolysis technologies are uncompetitive with low-cost grey hydrogen produced from fossil fuels, limiting their scale-up potential. Disruptive processes that decouple the hydrogen and oxygen evolution reactions and produce them in separate cells or different stages emerge as a prospective route to reduce system cost by enabling operation without expensive membranes and sealing components. Some of them divide the hydrogen or oxygen evolution reactions into electrochemical and chemical sub-reactions, leading the way to high efficiency. However, high efficiency was demonstrated only in a batch process with thermal swings that present operational challenges. This work introduces a breakthrough process that produces hydrogen and oxygen in separate cells and supports high-efficiency continuous operation in a membraneless system. We demonstrate high Faradaic and electrolytic efficiency and high-rate operation in a near-neutral electrolyte of NaBr in water.

Keywords

green hydrogen
electrolysis
decoupled water splitting
redox couple

Supplementary materials

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Supplementary information
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Supplementary data and results
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Video S1: Bromide electrolysis without stirring.
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Bromide electrolysis without stirring.
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Video S2: Stirring the oxidized electrolyte after bromide electrolysis.
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Stirring the oxidized electrolyte after bromide electrolysis (Video S1).
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Video S3: Iodometric titration.
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Iodometric titration to determine the conversion (Faradaic) efficiency in the bromide electrolysis experiment.
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Video S4a: Bromide electrolysis in a Hoffman apparatus; beginning.
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Bromide electrolysis in a Hoffman apparatus with the cathodic reaction on the left (HER) and anodic reaction on the right (bromide oxidation). (a) Beginning of the experiment.
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Video S4b: Bromide electrolysis in a Hoffman apparatus; middle.
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Bromide electrolysis in a Hoffman apparatus with the cathodic reaction on the left (HER) and anodic reaction on the right (bromide oxidation). (b) Middle of the experiment.
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Video S4c: Bromide electrolysis in a Hoffman apparatus; end.
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Bromide electrolysis in a Hoffman apparatus with the cathodic reaction on the left (HER) and anodic reaction on the right (bromide oxidation). (c) Ennd of the experiment.
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Video S5: Cataltytic bromate reduction.
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Catalytic bromate reduction and oxygen evolution.
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