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...

Full description

Saved in:
Bibliographic Details
Main Authors: Iwei Wang, Zhenshan Li
Format: Article
Language:English
Published: Elsevier 2024-12-01
Series:Carbon Capture Science & Technology
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S2772656824000733
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1850263790587740160
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.
format Article
id doaj-art-7ca771d88f354c9d987fea1d0be3c511
institution OA Journals
issn 2772-6568
language English
publishDate 2024-12-01
publisher Elsevier
record_format Article
series Carbon Capture Science & Technology
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