Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme
The integrated carbon capture and utilization (ICCU) technology, combined with the reverse water-gas shift reaction (RWGS), is considered a promising strategy for mitigating carbon emissions. This study investigates the limestone calcination and hydrogenation processes under relatively high partial...
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Elsevier
2024-12-01
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| Series: | Carbon Capture Science & Technology |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2772656824000733 |
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| author | Iwei Wang Zhenshan Li |
| author_facet | Iwei Wang Zhenshan Li |
| author_sort | Iwei Wang |
| collection | DOAJ |
| description | The integrated carbon capture and utilization (ICCU) technology, combined with the reverse water-gas shift reaction (RWGS), is considered a promising strategy for mitigating carbon emissions. This study investigates the limestone calcination and hydrogenation processes under relatively high partial pressures of CO2 in near-equilibrium conditions, at partial pressures (P) close to the equilibrium pressure (Peq), relevant to the ICCU-RWGS process, particularly during the in-situ CO2 conversion stage. The decomposition of CaCO3 during conventional calcination and hydrogenation under near-equilibrium conditions was initially examined using micro-fluidized bed thermogravimetric analysis coupled with mass spectrometry (MFB-TGA-MS) and a particle-injecting method. The results indicated that limestone decomposition during conventional calcination was inhibited under near-equilibrium conditions, with conversion near 0%. However, during the hydrogenation process, the interaction between H2 and CaCO3 further activated the decomposition of limestone. At 750 °C and P/Peq=0.9, limestone particles took ∼100 s to achieve complete conversion (100%). Given the known self-catalytic activity of CaO in converting carbonate to CO during hydrogenation, a dual-layer limestone hydrogenation process was further conducted using a fixed bed reactor. At 850 °C and a 30 vol.% H2 atmosphere, the limestone decomposition rate increased significantly and subsequently reacted with H2 to form CO, resulting in an H2/CO ratio of approximately 2.5. These findings support the viability of ICCU-RWGS approaches for future commercialization, with the product gas serving as the feedstock for the Fischer–Tropsch Synthesis (FTS) process. |
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| issn | 2772-6568 |
| language | English |
| publishDate | 2024-12-01 |
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| spelling | doaj-art-7ca771d88f354c9d987fea1d0be3c5112025-08-20T01:54:53ZengElsevierCarbon Capture Science & Technology2772-65682024-12-011310026110.1016/j.ccst.2024.100261Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization schemeIwei Wang0Zhenshan Li1Key Laboratory for Thermal Science and Power Engineering of the Ministry of Education, Department of Energy and Power Engineering, Tsinghua University, Beijing 100084, PR ChinaCorresponding author.; Key Laboratory for Thermal Science and Power Engineering of the Ministry of Education, Department of Energy and Power Engineering, Tsinghua University, Beijing 100084, PR ChinaThe integrated carbon capture and utilization (ICCU) technology, combined with the reverse water-gas shift reaction (RWGS), is considered a promising strategy for mitigating carbon emissions. This study investigates the limestone calcination and hydrogenation processes under relatively high partial pressures of CO2 in near-equilibrium conditions, at partial pressures (P) close to the equilibrium pressure (Peq), relevant to the ICCU-RWGS process, particularly during the in-situ CO2 conversion stage. The decomposition of CaCO3 during conventional calcination and hydrogenation under near-equilibrium conditions was initially examined using micro-fluidized bed thermogravimetric analysis coupled with mass spectrometry (MFB-TGA-MS) and a particle-injecting method. The results indicated that limestone decomposition during conventional calcination was inhibited under near-equilibrium conditions, with conversion near 0%. However, during the hydrogenation process, the interaction between H2 and CaCO3 further activated the decomposition of limestone. At 750 °C and P/Peq=0.9, limestone particles took ∼100 s to achieve complete conversion (100%). Given the known self-catalytic activity of CaO in converting carbonate to CO during hydrogenation, a dual-layer limestone hydrogenation process was further conducted using a fixed bed reactor. At 850 °C and a 30 vol.% H2 atmosphere, the limestone decomposition rate increased significantly and subsequently reacted with H2 to form CO, resulting in an H2/CO ratio of approximately 2.5. These findings support the viability of ICCU-RWGS approaches for future commercialization, with the product gas serving as the feedstock for the Fischer–Tropsch Synthesis (FTS) process.http://www.sciencedirect.com/science/article/pii/S2772656824000733Near-equilibriumCO2 partial pressurehydrogenationMFB-TGA-MSfixed bed |
| spellingShingle | Iwei Wang Zhenshan Li Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme Carbon Capture Science & Technology Near-equilibrium CO2 partial pressure hydrogenation MFB-TGA-MS fixed bed |
| title | Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme |
| title_full | Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme |
| title_fullStr | Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme |
| title_full_unstemmed | Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme |
| title_short | Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme |
| title_sort | near equilibrium analysis of co2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme |
| topic | Near-equilibrium CO2 partial pressure hydrogenation MFB-TGA-MS fixed bed |
| url | http://www.sciencedirect.com/science/article/pii/S2772656824000733 |
| work_keys_str_mv | AT iweiwang nearequilibriumanalysisofco2partialpressureoncarbonatehydrogenationinanintegratedcarboncaptureandutilizationscheme AT zhenshanli nearequilibriumanalysisofco2partialpressureoncarbonatehydrogenationinanintegratedcarboncaptureandutilizationscheme |