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Production of high purity H2 through chemical-looping water–gas shift at reforming temperatures – The importance of non-stoichiometric oxygen carriers

de Leeuwe, Christopher; Hu, Wenting; Evans, John; von Stosch, Moritz; Metcalfe, Ian S

Production of high purity H2 through chemical-looping water–gas shift at reforming temperatures – The importance of non-stoichiometric oxygen carriers Thumbnail


Authors

Christopher de Leeuwe

Wenting Hu

Moritz von Stosch

Ian S Metcalfe



Abstract

H2 is an important feedstock for many industrial processes and could be used as an energy carrier in a low carbon economy. This means that carbon neutral methods for H2 production are of vital importance. Chemical looping allows for H2 production with inherent carbon separation, making it an ideal system to produce low carbon H2. This work generates insights into the production of high purity H2 using a chemical looping packed bed reactor system containing an oxygen carrier of variable oxygen non-stoichiometry. Such a system has been shown to achieve 95% conversion of H2O to H2 at 1073 K outperforming the maximum theoretical conversions of 50% achieved by a conventional water gas shift reactor at that temperature. A numerical model was developed from theoretical consideration, with no fitted parameters and used to simulate the working reactor. Operando measurement of gas conversions and changes in solid oxygen capacity, through synchrotron X-ray diffraction, were used to validate the numerical model and confirmed that the reaction was thermodynamically limited. The model the model was shown to reproduce the conversion of the oxygen carrier, the reactant conversion and the product evolution. Sensitivity analysis showed that the relationship between the oxygen carrier material oxygen content and the chemical potential of oxygen in the carrier was the key consideration for the design and operation of a packed bed chemical looping reactor using an oxygen carrier of variable non-stoichiometry.

Citation

de Leeuwe, C., Hu, W., Evans, J., von Stosch, M., & Metcalfe, I. S. (2021). Production of high purity H2 through chemical-looping water–gas shift at reforming temperatures – The importance of non-stoichiometric oxygen carriers. Chemical Engineering Journal, 423, https://doi.org/10.1016/j.cej.2021.130174

Journal Article Type Article
Acceptance Date Apr 29, 2021
Online Publication Date May 7, 2021
Publication Date 2021
Deposit Date Aug 10, 2021
Publicly Available Date Aug 10, 2021
Journal Chemical Engineering Journal
Print ISSN 1385-8947
Publisher Elsevier
Peer Reviewed Peer Reviewed
Volume 423
DOI https://doi.org/10.1016/j.cej.2021.130174

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