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Separate H2 and CO production from CH4-CO2 cycling of Fe-Ni
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  • Bo Jin,
  • Nadadur Veeraraghavan Srinath,
  • Hilde Poelman,
  • Christophe Detavernier ,
  • Zhiwu Liang,
  • Guy Marin,
  • Vladimir Galvita
Bo Jin
Hunan University

Corresponding Author:[email protected]

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Nadadur Veeraraghavan Srinath
Ghent University
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Hilde Poelman
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Christophe Detavernier
Ghent University
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Zhiwu Liang
Joint International Center for CO2 Captu
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Guy Marin
Ghent University
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Vladimir Galvita
Universiteit Gent
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Abstract

Fe-Ni materials with varying Ni loading are developed for separate H2 and CO production by CH4-CO2 chemical looping. The product streams are obtained by first feeding CH4, which decomposes to H2 and carbon. The latter acts as reductant for the subsequent CO2 feed, which together with Fe re-oxidation yields CO. After 25 CH4-CO2 cycles, 10Fe5Ni@Zr has a higher H2 space-time-yield than 10Fe0Ni@Zr (〖20mmol∙s〗^(-1)∙kg_(Fe+Ni)^(-1) vs. 〖15mmol∙s〗^(-1)∙kg_(Fe+Ni)^(-1)), a 2.6 times higher CO (〖57mmol∙s〗^(-1)∙kg_(Fe+Ni)^(-1)) and lower deactivation. This improvement has two reasons: (i) CH4 activation over Ni leading to cracking, (ii) product hydrogen causing deeper FeO reduction. Deactivation follows from accumulated carbon, non-reactive for CO2. On Ni and Fe sites, carbon can be removed by lattice oxygen or CO2, yielding more CO compared to the theoretical value for Fe oxidation. However, carbon that migrates away from the metals requires oxygen for removal, which restores the activity of the Ni-containing samples.
29 Oct 2021Submitted to AIChE Journal
03 Nov 2021Submission Checks Completed
03 Nov 2021Assigned to Editor
20 Nov 2021Reviewer(s) Assigned
26 Jan 2022Editorial Decision: Revise Major
10 Mar 20221st Revision Received
16 Mar 2022Submission Checks Completed
16 Mar 2022Assigned to Editor
19 Mar 2022Reviewer(s) Assigned
09 May 2022Editorial Decision: Accept