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Title: Design and operational considerations of catalytic membrane reactors for ammonia synthesis

Abstract

Abstract Production of ammonia using hydrogen derived from renewable electricity instead of hydrocarbon reforming would dramatically reduce the carbon footprint of this commodity chemical. Novel technologies such as catalytic membrane reactors (CMRs) may potentially be more compatible with distributed ammonia production than the conventional Haber–Bosch process. A reactor model is developed based on integrating a standard industrial iron catalyst into a CMR equipped with an inorganic membrane that is selective to NH 3 over N 2 /H 2 . CMR performance is studied as functions of wide ranges of membrane properties and operating conditions. Conversion and ammonia recovery are dictated principally by the ammonia permeance, and the benefits by using membranes become significant above 100 GPU = 3.4 × 10 −8  mol m −2  s −1  Pa −1 . To be effective, the CMR requires a minimum selectivity for ammonia of 10 over both nitrogen and hydrogen and purity scales with the effective selectivity. Increasing the pressure of operation significantly improves all metrics, and at P  = 30 bar with a quality membrane, ammonia is almost completely recovered, enabling direct recycle of unreacted hydrogen and nitrogen without need for recompression. Temperature drives conversion and scales monotonically without thermodynamic limitations in a CMR. Alternatively, the temperature maymore » be reduced as low as 300°C while achieving conversion levels surpassing equilibrium limits at T  = 400°C in a conventional reactor.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Colorado School of Mines, Golden, CO (United States)
Publication Date:
Research Org.:
Colorado School of Mines, Golden, CO (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1779196
Alternate Identifier(s):
OSTI ID: 1786104
Grant/Contract Number:  
AR0001004
Resource Type:
Accepted Manuscript
Journal Name:
AIChE Journal
Additional Journal Information:
Journal Volume: 67; Journal Issue: 8; Journal ID: ISSN 0001-1541
Publisher:
American Institute of Chemical Engineers
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; membrane separations; process; reactor analysis; simulation

Citation Formats

Zhang, Zhenyu, Way, J. Douglas, and Wolden, Colin A. Design and operational considerations of catalytic membrane reactors for ammonia synthesis. United States: N. p., 2021. Web. doi:10.1002/aic.17259.
Zhang, Zhenyu, Way, J. Douglas, & Wolden, Colin A. Design and operational considerations of catalytic membrane reactors for ammonia synthesis. United States. https://doi.org/10.1002/aic.17259
Zhang, Zhenyu, Way, J. Douglas, and Wolden, Colin A. Mon . "Design and operational considerations of catalytic membrane reactors for ammonia synthesis". United States. https://doi.org/10.1002/aic.17259. https://www.osti.gov/servlets/purl/1779196.
@article{osti_1779196,
title = {Design and operational considerations of catalytic membrane reactors for ammonia synthesis},
author = {Zhang, Zhenyu and Way, J. Douglas and Wolden, Colin A.},
abstractNote = {Abstract Production of ammonia using hydrogen derived from renewable electricity instead of hydrocarbon reforming would dramatically reduce the carbon footprint of this commodity chemical. Novel technologies such as catalytic membrane reactors (CMRs) may potentially be more compatible with distributed ammonia production than the conventional Haber–Bosch process. A reactor model is developed based on integrating a standard industrial iron catalyst into a CMR equipped with an inorganic membrane that is selective to NH 3 over N 2 /H 2 . CMR performance is studied as functions of wide ranges of membrane properties and operating conditions. Conversion and ammonia recovery are dictated principally by the ammonia permeance, and the benefits by using membranes become significant above 100 GPU = 3.4 × 10 −8  mol m −2  s −1  Pa −1 . To be effective, the CMR requires a minimum selectivity for ammonia of 10 over both nitrogen and hydrogen and purity scales with the effective selectivity. Increasing the pressure of operation significantly improves all metrics, and at P  = 30 bar with a quality membrane, ammonia is almost completely recovered, enabling direct recycle of unreacted hydrogen and nitrogen without need for recompression. Temperature drives conversion and scales monotonically without thermodynamic limitations in a CMR. Alternatively, the temperature may be reduced as low as 300°C while achieving conversion levels surpassing equilibrium limits at T  = 400°C in a conventional reactor.},
doi = {10.1002/aic.17259},
journal = {AIChE Journal},
number = 8,
volume = 67,
place = {United States},
year = {Mon Mar 15 00:00:00 EDT 2021},
month = {Mon Mar 15 00:00:00 EDT 2021}
}

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