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Carbon-neutral and carbon-negative chemical looping processes using glycerol and methane as feedstock

Carbon-neutral and carbon-negative chemical looping processes using glycerol and methane as feedstock
Carbon-neutral and carbon-negative chemical looping processes using glycerol and methane as feedstock
Carbon-negative and neutral methods to produce H2 and other syngas-derived chemicals are tested and demonstrated in this study through chemical looping reforming of methane or glycerol. A chemical looping reactor provides the heat required to reform the glycerol or methane while having inherent CO2 capture. This is achieved using dynamically operated packed beds. If the glycerol or methane is from a biological source this gives the system the potential for negative emissions. To evaluate the potential of this system, 500 g packed bed of oxygen carriers were cyclically reduced, oxidized, and used to carry out reforming experiments. The reforming process was tested at various pressure (1 – 9 bar) and temperature (600 – 900 °C). These conditions were tested at this scale for the first time. Complete conversion of glycerol is achievable with only small quantities of CH4 slip. The maximum H2 production was achieved at 1 bar and 700 °C producing a H2/CO ratio of 10, this lowered to 9 when the temperature was increased to 900 °C. Adding CO2 to the feed stream along with H2O allows for a H2/CO ratio suitable for the Fischer Tropsch (FT) synthesis. Chemical looping reforming of CH4 with steam was successfully demonstrated in a lab reactor setup at 1 and 5 bar for multiple cycles with CH4 conversion > 99% and controlled heat losses. The temperature and concentration profiles provided identical results for consecutive cycles verifying the continuity and the feasibility of the process.
Chemical looping, Glycerol reforming, hydrogen, Negative emissions
0016-2361
de Leeuwe, Christopher
03e581bf-8436-4287-a9c0-9773c00cd541
Abbas, Syed Zaheer
3b02900e-fef6-40e1-acf7-96f26bfde4a8
Amieiro, Alvaro
82c4c3ed-2237-4191-9bda-c8b0eef5f8d2
Poulston, Stephen
74d12171-60ff-4566-847f-bbed3b76e0d0
Spallina, Vincenzo
e87fad8c-a44b-48a6-9da6-f60de3ce87a5
de Leeuwe, Christopher
03e581bf-8436-4287-a9c0-9773c00cd541
Abbas, Syed Zaheer
3b02900e-fef6-40e1-acf7-96f26bfde4a8
Amieiro, Alvaro
82c4c3ed-2237-4191-9bda-c8b0eef5f8d2
Poulston, Stephen
74d12171-60ff-4566-847f-bbed3b76e0d0
Spallina, Vincenzo
e87fad8c-a44b-48a6-9da6-f60de3ce87a5

de Leeuwe, Christopher, Abbas, Syed Zaheer, Amieiro, Alvaro, Poulston, Stephen and Spallina, Vincenzo (2023) Carbon-neutral and carbon-negative chemical looping processes using glycerol and methane as feedstock. Fuel, 353, [129001]. (doi:10.1016/j.fuel.2023.129001).

Record type: Article

Abstract

Carbon-negative and neutral methods to produce H2 and other syngas-derived chemicals are tested and demonstrated in this study through chemical looping reforming of methane or glycerol. A chemical looping reactor provides the heat required to reform the glycerol or methane while having inherent CO2 capture. This is achieved using dynamically operated packed beds. If the glycerol or methane is from a biological source this gives the system the potential for negative emissions. To evaluate the potential of this system, 500 g packed bed of oxygen carriers were cyclically reduced, oxidized, and used to carry out reforming experiments. The reforming process was tested at various pressure (1 – 9 bar) and temperature (600 – 900 °C). These conditions were tested at this scale for the first time. Complete conversion of glycerol is achievable with only small quantities of CH4 slip. The maximum H2 production was achieved at 1 bar and 700 °C producing a H2/CO ratio of 10, this lowered to 9 when the temperature was increased to 900 °C. Adding CO2 to the feed stream along with H2O allows for a H2/CO ratio suitable for the Fischer Tropsch (FT) synthesis. Chemical looping reforming of CH4 with steam was successfully demonstrated in a lab reactor setup at 1 and 5 bar for multiple cycles with CH4 conversion > 99% and controlled heat losses. The temperature and concentration profiles provided identical results for consecutive cycles verifying the continuity and the feasibility of the process.

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Accepted/In Press date: 11 June 2023
e-pub ahead of print date: 11 July 2023
Published date: 1 December 2023
Additional Information: Funding Information: The work has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement no. 884197 (GLAMOUR project). The work reflects only the authors' views and the EU is not liable for any use that may be made of the information contained therein. The authors acknowledge the Department of BEIS in the framework of the Low Carbon Hydrogen Supply 2: Stream 1 Phase 1 Competition (TRN 5044/04/2021) (RECYCLE, HYS2137) for providing funding and support to the development of this study. Funding Information: The work has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement no. 884197 (GLAMOUR project). The work reflects only the authors' views and the EU is not liable for any use that may be made of the information contained therein. The authors acknowledge the Department of BEIS in the framework of the Low Carbon Hydrogen Supply 2: Stream 1 Phase 1 Competition (TRN 5044/04/2021) (RECYCLE, HYS2137) for providing funding and support to the development of this study. Publisher Copyright: © 2023
Keywords: Chemical looping, Glycerol reforming, hydrogen, Negative emissions

Identifiers

Local EPrints ID: 481287
URI: http://eprints.soton.ac.uk/id/eprint/481287
ISSN: 0016-2361
PURE UUID: 6aea1825-6629-4a70-868e-ba6aa146c7c9
ORCID for Syed Zaheer Abbas: ORCID iD orcid.org/0000-0002-8783-8572

Catalogue record

Date deposited: 22 Aug 2023 16:41
Last modified: 17 Mar 2024 04:18

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Contributors

Author: Christopher de Leeuwe
Author: Syed Zaheer Abbas ORCID iD
Author: Alvaro Amieiro
Author: Stephen Poulston
Author: Vincenzo Spallina

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