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Title: Efficient Ammonia Decomposition in a Catalytic Membrane Reactor To Enable Hydrogen Storage and Utilization

Abstract

Liquid ammonia is a high density (17.7 wt. %) hydrogen carrier with a well-established production and distribution infrastructure. Efficient decomposition and purification are essential for its use as a hydrogen storage material. Here we demonstrate the production of high purity (> 99.7%) H 2 from NH 3 using a catalytic membrane reactor (CMR) in which a Ru catalyst is impregnated within a porous yttria-stabilized zirconia (YSZ) tube coated with a thin, 6 µm Pd film by electroless deposition. The intimate proximity of catalyst and membrane eliminates transport resistances that limit performance in the conventional packed bed membrane reactor (PBMR) configuration. The addition of a Cs promoter enabled complete NH 3 conversion at temperatures as low as 400°C, exceeding equilibrium constraints without the need for a sweep gas. A reactor model was developed that captured CMR performance with high fidelity. NH 3 decomposition was observed to follow first order kinetics due to efficient H 2 removal. Relative to a comparable PBMR, the Ru loading in the CMR was reduced an order of magnitude and the H 2 recovery increased 35%, enabling record volumetric productivity rates (> 30 mol m-3 s-1) that validate its promise for efficient, compact H 2 delivery frommore » ammonia.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Colorado School of Mines, Golden, CO (United States). Dept. of Chemical and Biological Engineering
Publication Date:
Research Org.:
Colorado School of Mines, Golden, CO (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Science Foundation (NSF)
OSTI Identifier:
1507121
Grant/Contract Number:  
AR0000785
Resource Type:
Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; Ammonia; Hydrogen; Membrane reactor; Model; Kinetics; Purification; Process intensification

Citation Formats

Zhang, Zhenyu, Liguori, Simona, Fuerst, Thomas F., Way, J. Douglas, and Wolden, Colin A. Efficient Ammonia Decomposition in a Catalytic Membrane Reactor To Enable Hydrogen Storage and Utilization. United States: N. p., 2019. Web. doi:10.1021/acssuschemeng.8b06065.
Zhang, Zhenyu, Liguori, Simona, Fuerst, Thomas F., Way, J. Douglas, & Wolden, Colin A. Efficient Ammonia Decomposition in a Catalytic Membrane Reactor To Enable Hydrogen Storage and Utilization. United States. doi:10.1021/acssuschemeng.8b06065.
Zhang, Zhenyu, Liguori, Simona, Fuerst, Thomas F., Way, J. Douglas, and Wolden, Colin A. Wed . "Efficient Ammonia Decomposition in a Catalytic Membrane Reactor To Enable Hydrogen Storage and Utilization". United States. doi:10.1021/acssuschemeng.8b06065.
@article{osti_1507121,
title = {Efficient Ammonia Decomposition in a Catalytic Membrane Reactor To Enable Hydrogen Storage and Utilization},
author = {Zhang, Zhenyu and Liguori, Simona and Fuerst, Thomas F. and Way, J. Douglas and Wolden, Colin A.},
abstractNote = {Liquid ammonia is a high density (17.7 wt. %) hydrogen carrier with a well-established production and distribution infrastructure. Efficient decomposition and purification are essential for its use as a hydrogen storage material. Here we demonstrate the production of high purity (> 99.7%) H2 from NH3 using a catalytic membrane reactor (CMR) in which a Ru catalyst is impregnated within a porous yttria-stabilized zirconia (YSZ) tube coated with a thin, 6 µm Pd film by electroless deposition. The intimate proximity of catalyst and membrane eliminates transport resistances that limit performance in the conventional packed bed membrane reactor (PBMR) configuration. The addition of a Cs promoter enabled complete NH3 conversion at temperatures as low as 400°C, exceeding equilibrium constraints without the need for a sweep gas. A reactor model was developed that captured CMR performance with high fidelity. NH3 decomposition was observed to follow first order kinetics due to efficient H2 removal. Relative to a comparable PBMR, the Ru loading in the CMR was reduced an order of magnitude and the H2 recovery increased 35%, enabling record volumetric productivity rates (> 30 mol m-3 s-1) that validate its promise for efficient, compact H2 delivery from ammonia.},
doi = {10.1021/acssuschemeng.8b06065},
journal = {ACS Sustainable Chemistry & Engineering},
number = 6,
volume = 7,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
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This content will become publicly available on February 27, 2020
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