期刊
NATURE CHEMISTRY
卷 11, 期 7, 页码 638-643出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-019-0273-2
关键词
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资金
- EPSRC
- European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013)/ERC grant [320725]
- EPSRC [EP/G012865/1, EP/J016454/1, EP/K029649/1, EP/P007767/1, EP/P024807/1]
- EPSRC [EP/P007767/1, EP/G012865/1, EP/K029649/1] Funding Source: UKRI
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-delta). 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.
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