Pub Date : 2025-09-04DOI: 10.1016/j.ccst.2025.100504
Néstor D. Montiel-Bohórquez, Manuele Gatti, Matteo C. Romano
This study presents a techno-economic analysis of four configurations of the Calcium Looping (CaL) technology, tailored to enhance system flexibility for capturing CO2 from the fluctuating flue gases generated by a scrap-based Electric Arc Furnace with a capacity of 112 tsteel/h. The configurations differ based on the solids circulation strategy between reactors (constant or variable) and the presence of one or two intermediate solids storage vessels. Configurations incorporating intermediate solids storage demonstrated operational advantages, including enhanced process stability and downsized calciner island components. Moreover, the plant configuration with two intermediate solids storages led to the lowest specific fuel consumption of 5.85 MJ per kgCO2 captured.
Under the assumptions considered, the CaL system achieved a CO2 capture rate of 91 % from the EAF off-gas. Moreover, using residual forestry biomass as fuel in the calciner enabled to achieve negative emissions with net CO2 removal rates of 13-26 tCO2/h, corresponding to 100-200 kgCO2 removed per tsteel produced.
From an economic standpoint, increment in steel cost ranged from 26 to 36 €/tsteel (assuming a carbon tax of 100 €/tCO2), with costs of CO2 avoided of 202-255 €/tCO2.
{"title":"Flexible calcium looping for CO2 capture in electric Arc Furnace steelmaking: A techno-economic analysis","authors":"Néstor D. Montiel-Bohórquez, Manuele Gatti, Matteo C. Romano","doi":"10.1016/j.ccst.2025.100504","DOIUrl":"10.1016/j.ccst.2025.100504","url":null,"abstract":"<div><div>This study presents a techno-economic analysis of four configurations of the Calcium Looping (CaL) technology, tailored to enhance system flexibility for capturing CO<sub>2</sub> from the fluctuating flue gases generated by a scrap-based Electric Arc Furnace with a capacity of 112 t<sub>steel</sub>/h. The configurations differ based on the solids circulation strategy between reactors (constant or variable) and the presence of one or two intermediate solids storage vessels. Configurations incorporating intermediate solids storage demonstrated operational advantages, including enhanced process stability and downsized calciner island components. Moreover, the plant configuration with two intermediate solids storages led to the lowest specific fuel consumption of 5.85 MJ per kg<sub>CO2</sub> captured.</div><div>Under the assumptions considered, the CaL system achieved a CO<sub>2</sub> capture rate of 91 % from the EAF off-gas. Moreover, using residual forestry biomass as fuel in the calciner enabled to achieve negative emissions with net CO<sub>2</sub> removal rates of 13-26 t<sub>CO2</sub>/h, corresponding to 100-200 kg<sub>CO2</sub> removed per t<sub>steel</sub> produced.</div><div>From an economic standpoint, increment in steel cost ranged from 26 to 36 €/t<sub>steel</sub> (assuming a carbon tax of 100 €/t<sub>CO2</sub>), with costs of CO<sub>2</sub> avoided of 202-255 €/t<sub>CO2</sub>.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100504"},"PeriodicalIF":0.0,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-01DOI: 10.1016/j.ccst.2025.100490
Liming Huang , Baodong Li , Xinping Zhu , Ning Li , Xin Zhang
Cement and concrete, while traditionally recognized as one of the main contributors to anthropogenic CO2 emissions, also have untapped capacity to serve as substantial carbon sinks. This paper provides a comprehensive perspective on how engineered mineral carbonation can transform cement-based materials into carbon storage systems. We briefly review the fundamental mechanisms of CO2 storage in cementitious systems and highlight current limitations in understanding of reaction kinetics, end-phase regulation and performance control. The effect of CO2 uptake on material performance is critically evaluated with respect to the fresh performance, mechanical properties and long-term durability. Emphasis is placed on the valorization of alkaline industrial residues and emerging carbonatable binders, which offer sequestration capacity and sustainable resource use. A strategic roadmap is proposed with integration of scientific innovation, regulatory alignment, and carbon accounting in the life cycle, to accelerate the adoption of carbon-storing concrete. This perspective provides a framework to advance cement and concrete as engineered carbon sinks and supports the transition to a climate-positive construction industry.
{"title":"Cement and concrete as carbon sinks: Transforming a climate challenge into a carbon storage opportunity","authors":"Liming Huang , Baodong Li , Xinping Zhu , Ning Li , Xin Zhang","doi":"10.1016/j.ccst.2025.100490","DOIUrl":"10.1016/j.ccst.2025.100490","url":null,"abstract":"<div><div>Cement and concrete, while traditionally recognized as one of the main contributors to anthropogenic CO<sub>2</sub> emissions, also have untapped capacity to serve as substantial carbon sinks. This paper provides a comprehensive perspective on how engineered mineral carbonation can transform cement-based materials into carbon storage systems. We briefly review the fundamental mechanisms of CO<sub>2</sub> storage in cementitious systems and highlight current limitations in understanding of reaction kinetics, end-phase regulation and performance control. The effect of CO<sub>2</sub> uptake on material performance is critically evaluated with respect to the fresh performance, mechanical properties and long-term durability. Emphasis is placed on the valorization of alkaline industrial residues and emerging carbonatable binders, which offer sequestration capacity and sustainable resource use. A strategic roadmap is proposed with integration of scientific innovation, regulatory alignment, and carbon accounting in the life cycle, to accelerate the adoption of carbon-storing concrete. This perspective provides a framework to advance cement and concrete as engineered carbon sinks and supports the transition to a climate-positive construction industry.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100490"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144921585","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-01DOI: 10.1016/j.ccst.2025.100503
Kamran Aghaee
Given the substantial share of global CO2 emissions attributable to construction materials, especially cement, there is rising interest in harnessing CO2 to enhance cementitious composites and generate value‑added products. Strategic carbon capture, utilization, and storage (CCUS) techniques including CO2 mixing, curing, and mineralization can improve the macro‑mechanical performance and microstructure of cement‑based materials and enable the development of novel binders and construction materials. This article synthesizes current CCUS techniques applicable to construction materials, particularly concrete composites, and elaborates on key parameters affecting their effectiveness. The findings suggest that CO2 mineralization is more effective than CO2 mixing and curing, revealing its considerable potential for producing carbon-sink materials from construction and industrial by-products that support circularity through reuse and closing the loop in construction. However, this approach still faces challenges related to scale-up and economic feasibility. This study compares and identifies the optimal implementation conditions to maximize material performance and production efficiency, while also evaluating the economic and environmental impacts of the technologies, with a focus on advancing circularity in construction.
{"title":"Carbon capture, utilization, and storage for sustainable construction: Insights into CO2 mixing, curing, and mineralization","authors":"Kamran Aghaee","doi":"10.1016/j.ccst.2025.100503","DOIUrl":"10.1016/j.ccst.2025.100503","url":null,"abstract":"<div><div>Given the substantial share of global CO<sub>2</sub> emissions attributable to construction materials, especially cement, there is rising interest in harnessing CO<sub>2</sub> to enhance cementitious composites and generate value‑added products. Strategic carbon capture, utilization, and storage (CCUS) techniques including CO<sub>2</sub> mixing, curing, and mineralization can improve the macro‑mechanical performance and microstructure of cement‑based materials and enable the development of novel binders and construction materials. This article synthesizes current CCUS techniques applicable to construction materials, particularly concrete composites, and elaborates on key parameters affecting their effectiveness. The findings suggest that CO<sub>2</sub> mineralization is more effective than CO<sub>2</sub> mixing and curing, revealing its considerable potential for producing carbon-sink materials from construction and industrial by-products that support circularity through reuse and closing the loop in construction. However, this approach still faces challenges related to scale-up and economic feasibility. This study compares and identifies the optimal implementation conditions to maximize material performance and production efficiency, while also evaluating the economic and environmental impacts of the technologies, with a focus on advancing circularity in construction.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100503"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-01DOI: 10.1016/j.ccst.2025.100476
Zengli Wang , Yaheng Pang , Xiao Wang , Hong Xu , Hongxia Guo , Li Liu , Haijun xu , Wenquan Cui , Xinying Liu
Global carbon emissions continue to rise, and carbon capture and utilization technologies have become a key path to carbon neutrality. The reverse water gas shift reaction (RWGS) has become a research hotspot in low-carbon conversion due to its ability to efficiently convert CO2 into CO and thereby synthesize high-value fuels and chemicals. However, it faces bottlenecks such as high energy consumption and poor low-temperature selectivity, which restrict its industrial application. This article systematically reviews the latest progress of RWGS reaction in the resource utilization of CO2, focusing on reaction mechanism, optimization of catalytic system, reactor innovation and breakthroughs in integrated technology. In the design of catalytic systems, electronic structure regulation, interface and defect engineering significantly enhance the CO2 conversion rate and product selectivity of thermal catalysis, photocatalysis and other systems. The reactor innovation breaks the thermodynamic equilibrium, optimizes mass transfer and overcomes thermodynamic limitations. The CO2 capture and conversion integrated technology, through the design of adsorption-catalytic dual-functional materials, couples capture and RWGS reactions, significantly reducing the separation energy consumption and transportation costs of traditional processes. Although there are still challenges in the stability of catalytic materials, adaptability to complex gas sources and large-scale application, in the future, focusing on the development of multifunctional materials, the coupling of clean energy and the analysis of dynamic reaction mechanisms will promote the practical application of RWGS technology in industrial carbon reduction.
{"title":"research progress on the optimization of RWGS catalytic systems and reactors and the integrated technology of CO2 capture and conversion","authors":"Zengli Wang , Yaheng Pang , Xiao Wang , Hong Xu , Hongxia Guo , Li Liu , Haijun xu , Wenquan Cui , Xinying Liu","doi":"10.1016/j.ccst.2025.100476","DOIUrl":"10.1016/j.ccst.2025.100476","url":null,"abstract":"<div><div>Global carbon emissions continue to rise, and carbon capture and utilization technologies have become a key path to carbon neutrality. The reverse water gas shift reaction (RWGS) has become a research hotspot in low-carbon conversion due to its ability to efficiently convert CO<sub>2</sub> into CO and thereby synthesize high-value fuels and chemicals. However, it faces bottlenecks such as high energy consumption and poor low-temperature selectivity, which restrict its industrial application. This article systematically reviews the latest progress of RWGS reaction in the resource utilization of CO<sub>2</sub>, focusing on reaction mechanism, optimization of catalytic system, reactor innovation and breakthroughs in integrated technology. In the design of catalytic systems, electronic structure regulation, interface and defect engineering significantly enhance the CO<sub>2</sub> conversion rate and product selectivity of thermal catalysis, photocatalysis and other systems. The reactor innovation breaks the thermodynamic equilibrium, optimizes mass transfer and overcomes thermodynamic limitations. The CO<sub>2</sub> capture and conversion integrated technology, through the design of adsorption-catalytic dual-functional materials, couples capture and RWGS reactions, significantly reducing the separation energy consumption and transportation costs of traditional processes. Although there are still challenges in the stability of catalytic materials, adaptability to complex gas sources and large-scale application, in the future, focusing on the development of multifunctional materials, the coupling of clean energy and the analysis of dynamic reaction mechanisms will promote the practical application of RWGS technology in industrial carbon reduction.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100476"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144921584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-01DOI: 10.1016/j.ccst.2025.100502
Wen-Long Xu , Tian-Ji Liu , Ya-Jun Wang , Ya-Nan Zeng , Liang-Yi Zhang , Kai-Li Dong , Yi-Tong Wang , Jun-Guo Li
The sustainable management of hazardous argon oxygen decarburization (AOD) slag demands urgent attention owing to its calcium-magnesium-silicon leaching risks in landfill scenarios. This study presents an innovative strategy for waste valorization by repurposing three modified AOD slag variants (raw, aged, and carbonated) as nutrient supplements for Chlorella pyrenoidosa cultivation. Moreover, process parameters in microalgae cultivation, such as algal characteristics and complex operational conditions, will affect its yield and productivity. Traditional methods struggle to enable comprehensive understanding and application. Thus, quantitative prediction was conducted using 96 sets of total CO2 carbon sequestration data (80% for the training set and 20% for the test set). Combined with three machine learning models and the Shapley Additive explanation (SHAP) algorithm, the intrinsic mechanisms by which five leaching elements (Ca, Mg, Al, Si, and Cr) regulate the efficient carbon sequestration of microalgae were analyzed. Notably, the random forest model excelled well in predicting CO2 storage and elemental leaching, with performance metrics exceeding 0.87. This approach integrating solid waste recycling, utilization and model development achieves three objectives: (1) establishing a circular economy pathway for metallurgical waste, (2) reducing microalgal cultivation costs through waste-derived nutrient substitution, and (3) providing a machine learning blueprint for hazardous waste valorization process optimization. The research results provide guidance for implementing a sustainable strategy of biocarbon capture while reducing industrial waste.
{"title":"Machine learning-driven optimization of argon oxygen decarburization slag recycling for enhanced microalgal carbon sequestration","authors":"Wen-Long Xu , Tian-Ji Liu , Ya-Jun Wang , Ya-Nan Zeng , Liang-Yi Zhang , Kai-Li Dong , Yi-Tong Wang , Jun-Guo Li","doi":"10.1016/j.ccst.2025.100502","DOIUrl":"10.1016/j.ccst.2025.100502","url":null,"abstract":"<div><div>The sustainable management of hazardous argon oxygen decarburization (AOD) slag demands urgent attention owing to its calcium-magnesium-silicon leaching risks in landfill scenarios. This study presents an innovative strategy for waste valorization by repurposing three modified AOD slag variants (raw, aged, and carbonated) as nutrient supplements for <em>Chlorella pyrenoidosa</em> cultivation. Moreover, process parameters in microalgae cultivation, such as algal characteristics and complex operational conditions, will affect its yield and productivity. Traditional methods struggle to enable comprehensive understanding and application. Thus, quantitative prediction was conducted using 96 sets of total CO<sub>2</sub> carbon sequestration data (80% for the training set and 20% for the test set). Combined with three machine learning models and the Shapley Additive explanation (SHAP) algorithm, the intrinsic mechanisms by which five leaching elements (Ca, Mg, Al, Si, and Cr) regulate the efficient carbon sequestration of microalgae were analyzed. Notably, the random forest model excelled well in predicting CO<sub>2</sub> storage and elemental leaching, with performance metrics exceeding 0.87. This approach integrating solid waste recycling, utilization and model development achieves three objectives: (1) establishing a circular economy pathway for metallurgical waste, (2) reducing microalgal cultivation costs through waste-derived nutrient substitution, and (3) providing a machine learning blueprint for hazardous waste valorization process optimization. The research results provide guidance for implementing a sustainable strategy of biocarbon capture while reducing industrial waste.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100502"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145046436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-30DOI: 10.1016/j.ccst.2025.100492
Yaozu Wang , Yuqi Niu , Yunrong Zhao , Bocheng Yu , Jinyang Xu , Yongqing Xu , Shijie Yu , Xuan Bie , Qinghai Li , Yanguo Zhang , Jingyuan Ma , Shuzhuang Sun , Fei Song , Hui Zhou
The incorporation of nitrate molten salts has been demonstrated as an effective strategy to enhance the CO2 uptake of MgO for intermediate-temperature (200–400 °C) CO2 capture. However, the slow carbonation kinetics in flue gas capture, coupled with poor stability, hinder its industrial application. In this study, the addition of Na2CO3 was found to significantly improve the sorption kinetics of MgO in a 15 % CO2 atmosphere, achieving a CO2 capacity of 19.9 mmol/g at 275 °C with a 15 mol% total promoter loading (Na2CO3/NaNO3 = 1:4). Mechanistic analysis revealed that Na2CO3 promotes the formation of Na2Mg(CO3)2, which acts as an effective nucleation site for MgCO3 formation, accelerating the carbonation rate by a factor of eight. The Hard X-ray photoelectron spectroscopy (HAXPES) revealed that an increased Na/Mg ratio caused subsurface migration and aggregation of molten salts, leading to a permanent rise in local salt concentrations, which negatively affected CO2 capture performance. These findings offer valuable insights into the structural degradation mechanisms and provide guidance for enhancing the stability of nitrate-enhanced MgO, thereby improving its potential for intermediate-temperature CO2 capture.
{"title":"Optimization and deactivation mechanisms of molten salt-promoted MgO for intermediate-temperature CO2 capture","authors":"Yaozu Wang , Yuqi Niu , Yunrong Zhao , Bocheng Yu , Jinyang Xu , Yongqing Xu , Shijie Yu , Xuan Bie , Qinghai Li , Yanguo Zhang , Jingyuan Ma , Shuzhuang Sun , Fei Song , Hui Zhou","doi":"10.1016/j.ccst.2025.100492","DOIUrl":"10.1016/j.ccst.2025.100492","url":null,"abstract":"<div><div>The incorporation of nitrate molten salts has been demonstrated as an effective strategy to enhance the CO<sub>2</sub> uptake of MgO for intermediate-temperature (200–400 °C) CO<sub>2</sub> capture. However, the slow carbonation kinetics in flue gas capture, coupled with poor stability, hinder its industrial application. In this study, the addition of Na<sub>2</sub>CO<sub>3</sub> was found to significantly improve the sorption kinetics of MgO in a 15 % CO<sub>2</sub> atmosphere, achieving a CO<sub>2</sub> capacity of 19.9 mmol/g at 275 °C with a 15 mol% total promoter loading (Na<sub>2</sub>CO<sub>3</sub>/NaNO<sub>3</sub> = 1:4). Mechanistic analysis revealed that Na<sub>2</sub>CO<sub>3</sub> promotes the formation of Na<sub>2</sub>Mg(CO<sub>3</sub>)<sub>2</sub>, which acts as an effective nucleation site for MgCO<sub>3</sub> formation, accelerating the carbonation rate by a factor of eight. The Hard X-ray photoelectron spectroscopy (HAXPES) revealed that an increased Na/Mg ratio caused subsurface migration and aggregation of molten salts, leading to a permanent rise in local salt concentrations, which negatively affected CO<sub>2</sub> capture performance. These findings offer valuable insights into the structural degradation mechanisms and provide guidance for enhancing the stability of nitrate-enhanced MgO, thereby improving its potential for intermediate-temperature CO<sub>2</sub> capture.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100492"},"PeriodicalIF":0.0,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145027387","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-28DOI: 10.1016/j.ccst.2025.100498
Luca Riboldi, Rahul Anantharaman, Donghoi Kim, Rubén M. Montañés, Simon Roussanaly, Sai Gokul Subraveti
There exists a portfolio of technologies that can be deployed for post-combustion CO2 capture. Each technology performs optimally at specific conditions, which will hardly coincide with exact industrial applications. Hybrid processes combine two (or more) technologies to perform the CO2 separation. The goal is to design processes that allow each technology in the hybrid configuration to operate optimally, resulting in cost-effective CO2 capture solutions. This study explores the feasibility of realizing this potential by mapping the techno-economic potential of selected hybrid processes across a wide spectrum of CO2 concentrations, plant scales and energy system contexts. The four hybrid processes considered are: vacuum pressure swing adsorption (VPSA)-membrane, membrane-VPSA, VPSA-CO2 liquefaction and membrane-CO2 liquefaction. A consistent techno-economic optimization framework is developed to identify the optimal process characteristics and associated minimum cost for each case considered. The performances are compared against those of conventional standalone capture technologies – VPSA, membranes and chemical absorption. Hybrid processes show promising results for medium-to-high CO2 concentrations (≈13–30 % CO2), where costs in the range 40–70 €/tCO2 appear achievable. However, even when different levels of electricity price and emission intensity are considered, chemical absorption and membranes remain the two most cost-efficient processes in most of the cases considered with hybrid processes at least 15 % more expensive. The material properties of membranes and adsorbents proved to have a significant impact on the expected performance. The sensitivity analysis showed how changing material properties assumption within relevant boundaries could modify the relative performance and advance hybrid processes, such as VPSA-membrane, as potentially attractive solutions, with the potential to decrease cost of >10 % at specific industrial conditions.
{"title":"Uncovering the opportunity space for hybrid CO₂ capture processes: A techno-economic exploration","authors":"Luca Riboldi, Rahul Anantharaman, Donghoi Kim, Rubén M. Montañés, Simon Roussanaly, Sai Gokul Subraveti","doi":"10.1016/j.ccst.2025.100498","DOIUrl":"10.1016/j.ccst.2025.100498","url":null,"abstract":"<div><div>There exists a portfolio of technologies that can be deployed for post-combustion CO<sub>2</sub> capture. Each technology performs optimally at specific conditions, which will hardly coincide with exact industrial applications. Hybrid processes combine two (or more) technologies to perform the CO<sub>2</sub> separation. The goal is to design processes that allow each technology in the hybrid configuration to operate optimally, resulting in cost-effective CO<sub>2</sub> capture solutions. This study explores the feasibility of realizing this potential by mapping the techno-economic potential of selected hybrid processes across a wide spectrum of CO<sub>2</sub> concentrations, plant scales and energy system contexts. The four hybrid processes considered are: vacuum pressure swing adsorption (VPSA)-membrane, membrane-VPSA, VPSA-CO<sub>2</sub> liquefaction and membrane-CO<sub>2</sub> liquefaction. A consistent techno-economic optimization framework is developed to identify the optimal process characteristics and associated minimum cost for each case considered. The performances are compared against those of conventional standalone capture technologies – VPSA, membranes and chemical absorption. Hybrid processes show promising results for medium-to-high CO<sub>2</sub> concentrations (≈13–30 % CO<sub>2</sub>), where costs in the range 40–70 €/t<sub>CO2</sub> appear achievable. However, even when different levels of electricity price and emission intensity are considered, chemical absorption and membranes remain the two most cost-efficient processes in most of the cases considered with hybrid processes at least 15 % more expensive. The material properties of membranes and adsorbents proved to have a significant impact on the expected performance. The sensitivity analysis showed how changing material properties assumption within relevant boundaries could modify the relative performance and advance hybrid processes, such as VPSA-membrane, as potentially attractive solutions, with the potential to decrease cost of >10 % at specific industrial conditions.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100498"},"PeriodicalIF":0.0,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145020148","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-28DOI: 10.1016/j.ccst.2025.100500
Hyeonji Yeom, Yongseok Kim, Woosung Leem, Jongmin Park, Kyungsu Na
The direct hydrogenation of CO2 using green hydrogen offers a sustainable route to produce carbon-neutral liquid hydrocarbons, emerging as a viable alternative to conventional naphtha cracking. Although Fe-based CuAl2O4 catalysts have been widely studied for CO2 hydrogenation, the mechanistic role of hydrogen spillover across dynamic Cu–Fe and associated oxygen vacancies has remained elusive. Here, the structure of FeK/CuAl2O4 catalysts was systematically tailored by controlling the reduction temperature to elucidate the exsolution-driven restructuration of pristine catalyst structure and its influences on the catalytic performance. We investigated the reaction process using in-situ DRIFTS analysis, from which we for the first time observed a cascade mechanism activated by hydrogen spillover, revealing various elementary reaction steps: (i) preferential adsorption of CO2 as carbonate species on oxygen vacancies created by Cu exsolution in CuAl2O4 lattice, (ii) effective formate-mediated reverse water–gas shift (RWGS) reaction via the hydrogen spillover from exsolved Cu, (iii) promoted Fischer–Tropsch synthesis (FTS) reaction on Fe5C2 formed by the facilitated Fe carburization at the exsolved Cu–Fe3O4 interfaces, (iv) rapid desorption of hydrocarbons produced via controlled carbon chain growth. This cooperative interaction enabled the selective production of C5–11 hydrocarbons, achieving the highest C5–11 productivity of 290.7 mL gcat–1 h–1, surpassing our previous work at a CO2 conversion of 36.4%. These findings establish a quantitative structure–performance–mechanism relationship and offer design principles for selectivity control toward desired hydrocarbon ranges in multifunctional CO2 hydrogenation catalysts.
使用绿色氢直接加氢二氧化碳为生产碳中性液态烃提供了一条可持续的途径，成为传统石脑油裂解的可行替代方案。虽然铁基CuAl2O4催化剂在CO2加氢中的应用已经得到了广泛的研究，但氢在Cu-Fe和伴生氧空位上的溢出机制仍然是一个谜。本研究通过控制还原温度，对FeK/CuAl2O4催化剂的结构进行了系统定制，以阐明析出驱动的原始催化剂结构重构及其对催化性能的影响。利用原位DRIFTS分析对反应过程进行了研究，首次观察到氢溢出激活的级联机制，揭示了不同的基本反应步骤：(1) Cu在CuAl2O4晶格中析出形成氧空位，CO2作为碳酸盐优先吸附；(2)通过析出Cu产生的氢溢出，甲酸介导的有效逆水气转换（RWGS）反应；(3)在析出Cu - fe3o4界面上促进Fe渗碳形成Fe5C2，促进了费托合成（FTS）反应；(4)通过控制碳链生长产生的碳氢化合物快速解吸。这种协同作用使C5-11碳氢化合物的选择性生产成为可能，达到了最高的C5-11产能290.7 mL gcat-1 h-1，超过了我们之前工作的36.4%的二氧化碳转化率。这些发现建立了定量的结构-性能-机理关系，并为多功能CO2加氢催化剂的选择性控制提供了设计原则。
{"title":"Mechanistic elucidation of cascade CO2 hydrogenation enabled by Cu–Fe interfaces and oxygen vacancies","authors":"Hyeonji Yeom, Yongseok Kim, Woosung Leem, Jongmin Park, Kyungsu Na","doi":"10.1016/j.ccst.2025.100500","DOIUrl":"10.1016/j.ccst.2025.100500","url":null,"abstract":"<div><div>The direct hydrogenation of CO<sub>2</sub> using green hydrogen offers a sustainable route to produce carbon-neutral liquid hydrocarbons, emerging as a viable alternative to conventional naphtha cracking. Although Fe-based CuAl<sub>2</sub>O<sub>4</sub> catalysts have been widely studied for CO<sub>2</sub> hydrogenation, the mechanistic role of hydrogen spillover across dynamic Cu–Fe and associated oxygen vacancies has remained elusive. Here, the structure of FeK/CuAl<sub>2</sub>O<sub>4</sub> catalysts was systematically tailored by controlling the reduction temperature to elucidate the exsolution-driven restructuration of pristine catalyst structure and its influences on the catalytic performance. We investigated the reaction process using in-situ DRIFTS analysis, from which we for the first time observed a cascade mechanism activated by hydrogen spillover, revealing various elementary reaction steps: (i) preferential adsorption of CO<sub>2</sub> as carbonate species on oxygen vacancies created by Cu exsolution in CuAl<sub>2</sub>O<sub>4</sub> lattice, (ii) effective formate-mediated reverse water–gas shift (RWGS) reaction via the hydrogen spillover from exsolved Cu, (iii) promoted Fischer–Tropsch synthesis (FTS) reaction on Fe<sub>5</sub>C<sub>2</sub> formed by the facilitated Fe carburization at the exsolved Cu–Fe<sub>3</sub>O<sub>4</sub> interfaces, (iv) rapid desorption of hydrocarbons produced via controlled carbon chain growth. This cooperative interaction enabled the selective production of C<sub>5–11</sub> hydrocarbons, achieving the highest C<sub>5–11</sub> productivity of 290.7 mL g<sub>cat</sub><sup>–1</sup> h<sup>–1</sup>, surpassing our previous work at a CO<sub>2</sub> conversion of 36.4%. These findings establish a quantitative structure–performance–mechanism relationship and offer design principles for selectivity control toward desired hydrocarbon ranges in multifunctional CO<sub>2</sub> hydrogenation catalysts.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100500"},"PeriodicalIF":0.0,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144933166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-27DOI: 10.1016/j.ccst.2025.100499
S. Mhlambi , O.E. Eruteya , F.A. Agbor , A. Moscariello , J.M. van Bever Donker , E. Samankassou
As global efforts to mitigate greenhouse gas emissions intensify, carbon capture and storage (CCS) has emerged as a key strategy for reducing the environmental impact of fossil fuel use. However, geological storage of CO₂ in structurally complex and heterogeneous reservoirs presents a range of issues due to the geological intricacies, with implications for storage capacity estimation, CO₂ injection, migration, and even long-term containment, which pose environmental risks. Therefore, this study assesses the CO₂ storage potential of the depleted F-O Gas Field in the Bredasdorp Basin, offshore South Africa, using a robust modelling approach based on the analysis of a suite of exploration and production datasets from the field. A high degree of structural compartmentalisation with a fault-bounded anticlinal trap characterises the field. The Valanginian-age marine sandstone reservoirs exhibit low to moderate porosity and permeability. In total, a CO₂ storage capacity of 185.3 Mt was determined for the F-O gas field, which reduces to 37.1–74.1 Mt after accounting for reservoir heterogeneity and sweep efficiency. This reduction reflects the impact of the field's complex structural architecture, variable facies distribution, and petrophysical variability, which collectively limit the effective pore volume accessible for CO2 storage. By rigorously integrating the structural architecture of the field, sedimentary processes, facies distribution, and petrophysical variability of the candidate reservoir, this study provides critical insights and strategies into the feasibility of CCS in structurally complex depleted gas fields. Significantly, these findings contribute to ongoing national CCS assessments and support South Africa’s long-term decarbonisation agenda.
{"title":"Assessing CO2 storage potential in a structurally complex depleted gas reservoir, offshore South Africa","authors":"S. Mhlambi , O.E. Eruteya , F.A. Agbor , A. Moscariello , J.M. van Bever Donker , E. Samankassou","doi":"10.1016/j.ccst.2025.100499","DOIUrl":"10.1016/j.ccst.2025.100499","url":null,"abstract":"<div><div>As global efforts to mitigate greenhouse gas emissions intensify, carbon capture and storage (CCS) has emerged as a key strategy for reducing the environmental impact of fossil fuel use. However, geological storage of CO₂ in structurally complex and heterogeneous reservoirs presents a range of issues due to the geological intricacies, with implications for storage capacity estimation, CO₂ injection, migration, and even long-term containment, which pose environmental risks. Therefore, this study assesses the CO₂ storage potential of the depleted F-O Gas Field in the Bredasdorp Basin, offshore South Africa, using a robust modelling approach based on the analysis of a suite of exploration and production datasets from the field. A high degree of structural compartmentalisation with a fault-bounded anticlinal trap characterises the field. The Valanginian-age marine sandstone reservoirs exhibit low to moderate porosity and permeability. In total, a CO₂ storage capacity of 185.3 Mt was determined for the F-O gas field, which reduces to 37.1–74.1 Mt after accounting for reservoir heterogeneity and sweep efficiency. This reduction reflects the impact of the field's complex structural architecture, variable facies distribution, and petrophysical variability, which collectively limit the effective pore volume accessible for CO<sub>2</sub> storage. By rigorously integrating the structural architecture of the field, sedimentary processes, facies distribution, and petrophysical variability of the candidate reservoir, this study provides critical insights and strategies into the feasibility of CCS in structurally complex depleted gas fields. Significantly, these findings contribute to ongoing national CCS assessments and support South Africa’s long-term decarbonisation agenda.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100499"},"PeriodicalIF":0.0,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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