High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor

Jose L. Cerrillo; Natalia Sanchez Morlanes; Shekhar Rajabhau Kulkarni; Natalia Realpe; Adrian Ramírez; Sai P. Katikaneni; Stephen N. Paglieri; Kunho Lee; Aadesh Harale; Bandar Solami; Aqil Jamal; Mani Sarathy; Pedro Castaño; Jorge Gascon

doi:10.1016/j.cej.2021.134310

High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor

Jose L. Cerrillo, Natalia Sanchez Morlanes, Shekhar Rajabhau Kulkarni, Natalia Realpe, Adrian Ramírez, Sai P. Katikaneni, Stephen N. Paglieri, Kunho Lee, Aadesh Harale, Bandar Solami, Aqil Jamal, Mani Sarathy, Pedro Castaño, Jorge Gascon

Research output: Contribution to journal › Article › peer-review

67 Scopus citations

Abstract

The combination of catalytic decomposition of ammonia and in situ separation of hydrogen holds great promise for the use of ammonia as a clean energy carrier. However, finding the optimal catalyst – membrane pair and operation conditions have proved challenging. Here, we demonstrate that cobalt-based catalysts for ammonia decomposition can be efficiently used together with a Pd-Au based membrane to produce high purity hydrogen at elevated pressure. Compared to a conventional packed bed reactor, the membrane reactor offers several operational advantages that result in energetic and economic benefits. The robustness and durability of the combined system has been demonstrated for>1000 h on stream, yielding a very pure hydrogen stream (>99.97 % H2) and recovery (>90 %). When considering the required hydrogen compression for storage/utilization and environmental issues, the combined system offers the additional advantage of production of hydrogen at moderate pressures along with full ammonia conversion. Altogether, our results demonstrate the possibility of deploying high pressure (350 bar) hydrogen generators from ammonia with H2 efficiencies of circa 75% without any external energy input and/or derived CO2 emissions.

Original language	English (US)
Pages (from-to)	134310
Journal	Chemical Engineering Journal
Volume	431
DOIs	https://doi.org/10.1016/j.cej.2021.134310
State	Published - Dec 24 2021

Bibliographical note

KAUST Repository Item: Exported on 2022-01-26
Acknowledgements: The authors gratefully acknowledge the financial support provided by Saudi Aramco, and the resources and facilities provided by the King Abdullah University of Science and Technology. N.M. and J.G. conceived this work. J.L.C and N.M. designed, characterized and conducted synthesis and catalytic experiments. N.R. and S.R.K. performed control regime studies. A.R. performed the technology simulation comparison and provided experimental support. J.G. P.C. and S.M.S. provided revision suggestions. J.L.C and N.M. wrote the original draft of the manuscript. All authors have given the approval to the final version of the manuscript.

ASJC Scopus subject areas

Environmental Chemistry
General Chemical Engineering
General Chemistry
Industrial and Manufacturing Engineering

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.cej.2021.134310

https://repository.kaust.edu.sa/bitstream/10754/675133/1/1-s2.0-S1385894721058824-main.pdf

Cite this

Cerrillo, J. L., Morlanes, N. S., Kulkarni, S. R., Realpe, N., Ramírez, A., Katikaneni, S. P., Paglieri, S. N., Lee, K., Harale, A., Solami, B., Jamal, A., Sarathy, M., Castaño, P., & Gascon, J. (2021). High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor. Chemical Engineering Journal, 431, 134310. https://doi.org/10.1016/j.cej.2021.134310

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title = "High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor",

abstract = "The combination of catalytic decomposition of ammonia and in situ separation of hydrogen holds great promise for the use of ammonia as a clean energy carrier. However, finding the optimal catalyst – membrane pair and operation conditions have proved challenging. Here, we demonstrate that cobalt-based catalysts for ammonia decomposition can be efficiently used together with a Pd-Au based membrane to produce high purity hydrogen at elevated pressure. Compared to a conventional packed bed reactor, the membrane reactor offers several operational advantages that result in energetic and economic benefits. The robustness and durability of the combined system has been demonstrated for>1000 h on stream, yielding a very pure hydrogen stream (>99.97 % H2) and recovery (>90 %). When considering the required hydrogen compression for storage/utilization and environmental issues, the combined system offers the additional advantage of production of hydrogen at moderate pressures along with full ammonia conversion. Altogether, our results demonstrate the possibility of deploying high pressure (350 bar) hydrogen generators from ammonia with H2 efficiencies of circa 75% without any external energy input and/or derived CO2 emissions.",

author = "Cerrillo, {Jose L.} and Morlanes, {Natalia Sanchez} and Kulkarni, {Shekhar Rajabhau} and Natalia Realpe and Adrian Ram{\'i}rez and Katikaneni, {Sai P.} and Paglieri, {Stephen N.} and Kunho Lee and Aadesh Harale and Bandar Solami and Aqil Jamal and Mani Sarathy and Pedro Casta{\~n}o and Jorge Gascon",

note = "KAUST Repository Item: Exported on 2022-01-26 Acknowledgements: The authors gratefully acknowledge the financial support provided by Saudi Aramco, and the resources and facilities provided by the King Abdullah University of Science and Technology. N.M. and J.G. conceived this work. J.L.C and N.M. designed, characterized and conducted synthesis and catalytic experiments. N.R. and S.R.K. performed control regime studies. A.R. performed the technology simulation comparison and provided experimental support. J.G. P.C. and S.M.S. provided revision suggestions. J.L.C and N.M. wrote the original draft of the manuscript. All authors have given the approval to the final version of the manuscript.",

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Cerrillo, JL, Morlanes, NS , Kulkarni, SR , Realpe, N, Ramírez, A, Katikaneni, SP, Paglieri, SN, Lee, K, Harale, A, Solami, B, Jamal, A, Sarathy, M , Castaño, P & Gascon, J 2021, 'High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor', Chemical Engineering Journal, vol. 431, pp. 134310. https://doi.org/10.1016/j.cej.2021.134310

TY - JOUR

T1 - High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor

AU - Cerrillo, Jose L.

AU - Morlanes, Natalia Sanchez

AU - Kulkarni, Shekhar Rajabhau

AU - Realpe, Natalia

AU - Ramírez, Adrian

AU - Katikaneni, Sai P.

AU - Paglieri, Stephen N.

AU - Lee, Kunho

AU - Harale, Aadesh

AU - Solami, Bandar

AU - Jamal, Aqil

AU - Sarathy, Mani

AU - Castaño, Pedro

AU - Gascon, Jorge

N1 - KAUST Repository Item: Exported on 2022-01-26 Acknowledgements: The authors gratefully acknowledge the financial support provided by Saudi Aramco, and the resources and facilities provided by the King Abdullah University of Science and Technology. N.M. and J.G. conceived this work. J.L.C and N.M. designed, characterized and conducted synthesis and catalytic experiments. N.R. and S.R.K. performed control regime studies. A.R. performed the technology simulation comparison and provided experimental support. J.G. P.C. and S.M.S. provided revision suggestions. J.L.C and N.M. wrote the original draft of the manuscript. All authors have given the approval to the final version of the manuscript.

PY - 2021/12/24

Y1 - 2021/12/24

N2 - The combination of catalytic decomposition of ammonia and in situ separation of hydrogen holds great promise for the use of ammonia as a clean energy carrier. However, finding the optimal catalyst – membrane pair and operation conditions have proved challenging. Here, we demonstrate that cobalt-based catalysts for ammonia decomposition can be efficiently used together with a Pd-Au based membrane to produce high purity hydrogen at elevated pressure. Compared to a conventional packed bed reactor, the membrane reactor offers several operational advantages that result in energetic and economic benefits. The robustness and durability of the combined system has been demonstrated for>1000 h on stream, yielding a very pure hydrogen stream (>99.97 % H2) and recovery (>90 %). When considering the required hydrogen compression for storage/utilization and environmental issues, the combined system offers the additional advantage of production of hydrogen at moderate pressures along with full ammonia conversion. Altogether, our results demonstrate the possibility of deploying high pressure (350 bar) hydrogen generators from ammonia with H2 efficiencies of circa 75% without any external energy input and/or derived CO2 emissions.

AB - The combination of catalytic decomposition of ammonia and in situ separation of hydrogen holds great promise for the use of ammonia as a clean energy carrier. However, finding the optimal catalyst – membrane pair and operation conditions have proved challenging. Here, we demonstrate that cobalt-based catalysts for ammonia decomposition can be efficiently used together with a Pd-Au based membrane to produce high purity hydrogen at elevated pressure. Compared to a conventional packed bed reactor, the membrane reactor offers several operational advantages that result in energetic and economic benefits. The robustness and durability of the combined system has been demonstrated for>1000 h on stream, yielding a very pure hydrogen stream (>99.97 % H2) and recovery (>90 %). When considering the required hydrogen compression for storage/utilization and environmental issues, the combined system offers the additional advantage of production of hydrogen at moderate pressures along with full ammonia conversion. Altogether, our results demonstrate the possibility of deploying high pressure (350 bar) hydrogen generators from ammonia with H2 efficiencies of circa 75% without any external energy input and/or derived CO2 emissions.

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U2 - 10.1016/j.cej.2021.134310

DO - 10.1016/j.cej.2021.134310

M3 - Article

SN - 1385-8947

VL - 431

SP - 134310

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

ER -

High purity, self-sustained, pressurized hydrogen production from ammonia in a catalytic membrane reactor

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

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