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Overcoming chemical equilibrium limitations using a thermodynamically reversible chemical reactor

Metcalfe, Ian S.; Ray, Brian; Dejoie, Catherine; Hu, Wenting; de Leeuwe, Christopher; Dueso, Cristina; García-García, Francisco R.; Mak, Cheuk-Man; Papaioannou, Evangelos I.; Thompson, Claire R.; Evans, John S.O.

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Authors

Ian S. Metcalfe

Brian Ray

Catherine Dejoie

Wenting Hu

Christopher de Leeuwe

Cristina Dueso

Francisco R. García-García

Cheuk-Man Mak

Evangelos I. Papaioannou

Claire R. Thompson



Abstract

All real processes, be they chemical, mechanical or electrical, are thermodynamically irreversible and therefore suffer from thermodynamic losses. Here, we report the design and operation of a chemical reactor capable of approaching thermodynamically reversible operation. The reactor was employed for hydrogen production via the water–gas shift reaction, an important route to ‘green’ hydrogen. The reactor avoids mixing reactant gases by transferring oxygen from the (oxidizing) water stream to the (reducing) carbon monoxide stream via a solid-state oxygen reservoir consisting of a perovskite phase (La0.6Sr0.4FeO3-δ). This reservoir is able to remain close to equilibrium with the reacting gas streams because of its variable degree of non-stoichiometry and thus develops a ‘chemical memory’ that we employ to approach reversibility. We demonstrate this memory using operando, spatially resolved, real-time, high-resolution X-ray powder diffraction on a working reactor. The design leads to a reactor unconstrained by overall chemical equilibrium limitations, which can produce essentially pure hydrogen and carbon dioxide as separate product streams.

Citation

Metcalfe, I. S., Ray, B., Dejoie, C., Hu, W., de Leeuwe, C., Dueso, C., …Evans, J. S. (2019). Overcoming chemical equilibrium limitations using a thermodynamically reversible chemical reactor. Nature Chemistry, 11, 638-643. https://doi.org/10.1038/s41557-019-0273-2

Journal Article Type Article
Acceptance Date Apr 17, 2019
Online Publication Date May 27, 2019
Publication Date 2019
Deposit Date Jun 5, 2019
Publicly Available Date Nov 27, 2019
Journal Nature Chemistry
Print ISSN 1755-4330
Electronic ISSN 1755-4349
Publisher Nature Research
Peer Reviewed Peer Reviewed
Volume 11
Pages 638-643
DOI https://doi.org/10.1038/s41557-019-0273-2
Public URL https://durham-repository.worktribe.com/output/1300470

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