Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ
NH3 and CO2 can react to produce syngas (H2 + CO), which serves as a feedstock for the production of chemicals or synthetic fuels. Combining NH3 cracking (NH3 → 0.5N2 + 1.5H2) and the redox-mediated reverse water gas shift reaction (RWGS, CO2 + H2 → CO + H2O), we propose the “NH3-RWGS” process in a...
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Elsevier
2025-05-01
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2666821125000109 |
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| author | Martin Keller Shih-Yuan Chen Atul Sharma |
| author_facet | Martin Keller Shih-Yuan Chen Atul Sharma |
| author_sort | Martin Keller |
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| description | NH3 and CO2 can react to produce syngas (H2 + CO), which serves as a feedstock for the production of chemicals or synthetic fuels. Combining NH3 cracking (NH3 → 0.5N2 + 1.5H2) and the redox-mediated reverse water gas shift reaction (RWGS, CO2 + H2 → CO + H2O), we propose the “NH3-RWGS” process in a two-reactor system that can produce N2-free syngas without requiring a downstream gas separation step. We investigate the role of La0.75Sr0.25Cr0.5Mn0.5O3−δ (LSCM) in the redox-mediated RWGS, combined with a stabilized Ni catalyst to impart NH3 cracking functionality. The mixture of LSCM and Ni catalyst at a weight ratio of 10:1 increases the NH3 cracking activity fivefold compared to using only LSCM. Because the reduction of LSCM proceeds through a two-step mechanism that requires the prior cracking of NH3, it also substantially increases the redox reactivity of LSCM. The Ni catalyst exhibits undesirable nitrogen uptake at ∼500 °C, and the redox capacity of LSCM with NH3 and CO2 decreases with temperature. Therefore, the process is best implemented at ∼600 °C. Under these conditions, the application of the “NH3-RWGS” process with mixtures of LSCM and Ni catalyst is promising to produce high-quality, N2-free syngas directly from NH3 and CO2. |
| format | Article |
| id | doaj-art-9c665c43e56647f98644cbcdb5f393d6 |
| institution | Kabale University |
| issn | 2666-8211 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Elsevier |
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| spelling | doaj-art-9c665c43e56647f98644cbcdb5f393d62025-02-10T04:35:01ZengElsevierChemical Engineering Journal Advances2666-82112025-05-0122100713Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δMartin Keller0Shih-Yuan Chen1Atul Sharma2National Institute of Advanced Industrial Science and Technology, Global Zero Emission Research Center, Smart CO2 Utilization Research Team, 16-1, Onogawa, Tsukuba, Ibaraki 305-8569, Japan; Corresponding author.National Institute of Advanced Industrial Science and Technology, Energy Catalyst Technology Group, Energy Process Research Institute (EPRI), 16-1, Onogawa, Tsukuba, Ibaraki 305-8569, JapanNational Institute of Advanced Industrial Science and Technology, Global Zero Emission Research Center, Smart CO2 Utilization Research Team, 16-1, Onogawa, Tsukuba, Ibaraki 305-8569, JapanNH3 and CO2 can react to produce syngas (H2 + CO), which serves as a feedstock for the production of chemicals or synthetic fuels. Combining NH3 cracking (NH3 → 0.5N2 + 1.5H2) and the redox-mediated reverse water gas shift reaction (RWGS, CO2 + H2 → CO + H2O), we propose the “NH3-RWGS” process in a two-reactor system that can produce N2-free syngas without requiring a downstream gas separation step. We investigate the role of La0.75Sr0.25Cr0.5Mn0.5O3−δ (LSCM) in the redox-mediated RWGS, combined with a stabilized Ni catalyst to impart NH3 cracking functionality. The mixture of LSCM and Ni catalyst at a weight ratio of 10:1 increases the NH3 cracking activity fivefold compared to using only LSCM. Because the reduction of LSCM proceeds through a two-step mechanism that requires the prior cracking of NH3, it also substantially increases the redox reactivity of LSCM. The Ni catalyst exhibits undesirable nitrogen uptake at ∼500 °C, and the redox capacity of LSCM with NH3 and CO2 decreases with temperature. Therefore, the process is best implemented at ∼600 °C. Under these conditions, the application of the “NH3-RWGS” process with mixtures of LSCM and Ni catalyst is promising to produce high-quality, N2-free syngas directly from NH3 and CO2.http://www.sciencedirect.com/science/article/pii/S2666821125000109NH3 crackingReverse water gas shiftCO2 utilizationChemical loopingSyngas production |
| spellingShingle | Martin Keller Shih-Yuan Chen Atul Sharma Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ Chemical Engineering Journal Advances NH3 cracking Reverse water gas shift CO2 utilization Chemical looping Syngas production |
| title | Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ |
| title_full | Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ |
| title_fullStr | Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ |
| title_full_unstemmed | Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ |
| title_short | Redox-mediated reverse water gas shift integrated with ammonia cracking over Ni/La0.75Sr0.25Cr0.5Mn0.5O3−δ |
| title_sort | redox mediated reverse water gas shift integrated with ammonia cracking over ni la0 75sr0 25cr0 5mn0 5o3 δ |
| topic | NH3 cracking Reverse water gas shift CO2 utilization Chemical looping Syngas production |
| url | http://www.sciencedirect.com/science/article/pii/S2666821125000109 |
| work_keys_str_mv | AT martinkeller redoxmediatedreversewatergasshiftintegratedwithammoniacrackingovernila075sr025cr05mn05o3d AT shihyuanchen redoxmediatedreversewatergasshiftintegratedwithammoniacrackingovernila075sr025cr05mn05o3d AT atulsharma redoxmediatedreversewatergasshiftintegratedwithammoniacrackingovernila075sr025cr05mn05o3d |