Pub Date : 2025-12-01Epub Date: 2025-09-22DOI: 10.1016/j.ccst.2025.100522
Jian Shen , Chaoxing Li , Yongqi Liu , Mingliang Yang , Qiongzhi Zhou , Fei Kang , Xiaohong Zheng , He Zhao , Sandip Sabale , Deok-kee Kim , Yiming Li , Jian Xiong , Qiangying Zhang , Yu Zheng
The utilization or emission of fluorocarbons in varied industries, including fine chemicals development, nonferrous metals smelting, electronics/semiconductors fabrication, and space heating/cooling, is continuously increasing year after year due to society advancement and population expansion, but at the prices of chemicals waste and irreversible environmental issues. Thus, the development of engineered solid sorbents will necessitate the capture, separation, and recycling of fluorocarbons in each scenario. This review initially discusses the sources and techniques required for various fluorocarbons used or emitted in existing industries, followed by a brief introduction to the importances of sorption media. The impacts of sorbents used in fluorocarbon sorption-related applications are reviewed to emphasize the importance of engineered nanoporous sorbents with specific textural/chemical properties to improve sorption-related performance. Furthermore, engineered strategies for sorbent design based on continuous pore-filling mechanisms, including sorbent-fluorocarbons interactions by controlling the strength of acid-base pairs and fluorocarbon-fluorocarbon interactions by tuning pore size/dimension/shape/morphology, are outlined. In addition, systemic experimental and computational characterizations provide insights into structure-performance correlations and corresponding sorption mechanisms. Next, we exemplified perfluorocarbons and refrigerants as typical fluorocarbons to further illustrate the roles of engineered nanoporous sorbents in fluorocarbon sorption performance. Finally, we emphasize the future challenges and opportunities for fluorinated gas purification and reuse with the “Mechanisms—Data” dual-driven conception for engineered nanoporous sorbent development.
{"title":"Engineered nanoporous sorbents for gaseous fluorocarbons related adsorption applications","authors":"Jian Shen , Chaoxing Li , Yongqi Liu , Mingliang Yang , Qiongzhi Zhou , Fei Kang , Xiaohong Zheng , He Zhao , Sandip Sabale , Deok-kee Kim , Yiming Li , Jian Xiong , Qiangying Zhang , Yu Zheng","doi":"10.1016/j.ccst.2025.100522","DOIUrl":"10.1016/j.ccst.2025.100522","url":null,"abstract":"<div><div>The utilization or emission of fluorocarbons in varied industries, including fine chemicals development, nonferrous metals smelting, electronics/semiconductors fabrication, and space heating/cooling, is continuously increasing year after year due to society advancement and population expansion, but at the prices of chemicals waste and irreversible environmental issues. Thus, the development of engineered solid sorbents will necessitate the capture, separation, and recycling of fluorocarbons in each scenario. This review initially discusses the sources and techniques required for various fluorocarbons used or emitted in existing industries, followed by a brief introduction to the importances of sorption media. The impacts of sorbents used in fluorocarbon sorption-related applications are reviewed to emphasize the importance of engineered nanoporous sorbents with specific textural/chemical properties to improve sorption-related performance. Furthermore, engineered strategies for sorbent design based on continuous pore-filling mechanisms, including sorbent-fluorocarbons interactions by controlling the strength of acid-base pairs and fluorocarbon-fluorocarbon interactions by tuning pore size/dimension/shape/morphology, are outlined. In addition, systemic experimental and computational characterizations provide insights into structure-performance correlations and corresponding sorption mechanisms. Next, we exemplified perfluorocarbons and refrigerants as typical fluorocarbons to further illustrate the roles of engineered nanoporous sorbents in fluorocarbon sorption performance. Finally, we emphasize the future challenges and opportunities for fluorinated gas purification and reuse with the “Mechanisms—Data” dual-driven conception for engineered nanoporous sorbent development.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100522"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145155275","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 : 2025-12-01Epub Date: 2025-09-04DOI: 10.1016/j.ccst.2025.100510
Andrea Pierozzi , Niamh Faulkner , Adrienn Maria Szucs , Luca Terribili , Melanie Maddin , Federica Meloni , Kavya Devkota , Kristina Petra Zubovic , Paul C. Guyett , Juan Diego Rodriguez-Blanco
This study investigates hydrothermal carbonate cements in Quaternary alkali basalts from the Sverrefjellet volcano (Svalbard), offering insights into in-situ natural mineral carbonation. XRD and SEM-BSE-EDS analyses identify two main morphologies, nodular and banded, composed of solid-solution series between magnesite, calcite, and siderite, with distinct compositional zonation. Nodular cements usually show concentric zoning from Mg-rich cores (Ca0.05Mg0.95CO3) to Ca-enriched rims (Ca0.40Mg0.60CO3), reflecting evolving fluid chemistry. Fe-rich nodules (Ca0.10Mg0.50Fe0.40CO3) are found near pyrite and display dissolution textures linked to localized redox reactions. Banded cements initiate at the basalt interface as Ca-rich proto-dolomite (Ca0.65–0.58Mg0.35–0.42CO3), transitioning outward to magnesite (Ca0.10Mg0.90CO3) and ferroan magnesite (Ca0.10Mg0.50Fe0.40CO3). Ca/Mg ratios decrease with distance from the interface (1.81 to 0.13), while Fe/Mg exceeds 13.5 locally due to Fe-rich coatings and inclusions. Four sequential crystallization stages were identified: (1) irregularly laminated Ca-Mg carbonates, (2) oscillatory-zoned dolomite-magnesite, (3) radiaxial-fibrous Ca-bearing magnesite, and (4) Fe-oxide-rich nanocrystalline rinds. Basaltic silicate and glass dissolution (forsterite, enstatite, anorthite) supplied divalent cations. Redox shifts promoted Fe incorporation. Early Ca2+ depletion altered fluid chemistry toward Mg2+ and Fe2+, while oscillatory zoning reflects episodic fluid compositional variations. Pyrite and siderite dissolution imply late-stage oxidation and secondary porosity development. These carbonates are hydrothermal in origin, supported by high-temperature phases, fan-like growth textures, and Ca-to-Mg/Fe transitions, consistent with fluid-rock interaction at 60–220 °C and pH 5.2–6.5. The absence of hydrated carbonates and presence of alteration phases also supports hydrothermal precipitation. Comparisons with engineered systems (e.g., CarbFix) underscore the role of temperature in overcoming kinetic barriers to magnesite formation, though metastable proto-dolomite and Mg sequestration in clays reveal limits to carbonation efficiency. These findings constrain predictive models for CO2 mineralization in basaltic reservoirs, highlighting the interplay of hydrothermal conditions, fluid evolution, and reaction kinetics.
{"title":"Natural carbonation in alkali basalts: Geochemical evolution of Ca–Mg–Fe carbonates at Sverrefjellet, Svalbard","authors":"Andrea Pierozzi , Niamh Faulkner , Adrienn Maria Szucs , Luca Terribili , Melanie Maddin , Federica Meloni , Kavya Devkota , Kristina Petra Zubovic , Paul C. Guyett , Juan Diego Rodriguez-Blanco","doi":"10.1016/j.ccst.2025.100510","DOIUrl":"10.1016/j.ccst.2025.100510","url":null,"abstract":"<div><div>This study investigates hydrothermal carbonate cements in Quaternary alkali basalts from the Sverrefjellet volcano (Svalbard), offering insights into in-situ natural mineral carbonation. XRD and SEM-BSE-EDS analyses identify two main morphologies, nodular and banded, composed of solid-solution series between magnesite, calcite, and siderite, with distinct compositional zonation. Nodular cements usually show concentric zoning from Mg-rich cores (Ca<sub>0.05</sub>Mg<sub>0.95</sub>CO<sub>3</sub>) to Ca-enriched rims (Ca<sub>0.40</sub>Mg<sub>0.60</sub>CO<sub>3</sub>), reflecting evolving fluid chemistry. Fe-rich nodules (Ca<sub>0.10</sub>Mg<sub>0.50</sub>Fe<sub>0.40</sub>CO<sub>3</sub>) are found near pyrite and display dissolution textures linked to localized redox reactions. Banded cements initiate at the basalt interface as Ca-rich proto-dolomite (Ca<sub>0.65–0.58</sub>Mg<sub>0.35–0.42</sub>CO<sub>3</sub>), transitioning outward to magnesite (Ca<sub>0.10</sub>Mg<sub>0.90</sub>CO<sub>3</sub>) and ferroan magnesite (Ca<sub>0.10</sub>Mg<sub>0.50</sub>Fe<sub>0.40</sub>CO<sub>3</sub>). Ca/Mg ratios decrease with distance from the interface (1.81 to 0.13), while Fe/Mg exceeds 13.5 locally due to Fe-rich coatings and inclusions. Four sequential crystallization stages were identified: (1) irregularly laminated Ca-Mg carbonates, (2) oscillatory-zoned dolomite-magnesite, (3) radiaxial-fibrous Ca-bearing magnesite, and (4) Fe-oxide-rich nanocrystalline rinds. Basaltic silicate and glass dissolution (forsterite, enstatite, anorthite) supplied divalent cations. Redox shifts promoted Fe incorporation. Early Ca<sup>2+</sup> depletion altered fluid chemistry toward Mg<sup>2+</sup> and Fe<sup>2+</sup>, while oscillatory zoning reflects episodic fluid compositional variations. Pyrite and siderite dissolution imply late-stage oxidation and secondary porosity development. These carbonates are hydrothermal in origin, supported by high-temperature phases, fan-like growth textures, and Ca-to-Mg/Fe transitions, consistent with fluid-rock interaction at 60–220 °C and pH 5.2–6.5. The absence of hydrated carbonates and presence of alteration phases also supports hydrothermal precipitation. Comparisons with engineered systems (e.g., CarbFix) underscore the role of temperature in overcoming kinetic barriers to magnesite formation, though metastable proto-dolomite and Mg sequestration in clays reveal limits to carbonation efficiency. These findings constrain predictive models for CO<sub>2</sub> mineralization in basaltic reservoirs, highlighting the interplay of hydrothermal conditions, fluid evolution, and reaction kinetics.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100510"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145027390","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 : 2025-12-01Epub 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":"2025-12-01","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 : 2025-12-01Epub Date: 2025-09-26DOI: 10.1016/j.ccst.2025.100524
Zikir A. Kemala , Manav Kakkanat , Andrey G. Kalinichev , Narasimhan Loganathan , Juliana Zaini , Malik M. Nauman , A. Ozgur Yazaydin
The long-term security of geological CO₂ storage depends not only on the capacity of reservoir rocks to accommodate CO₂ but also on their ability to retain it under leakage scenarios. In this study, molecular dynamics simulations were used to investigate CO₂ behavior in illite-based shale pores with varying organic content and structural configurations. Three representative pore models were examined: a purely mineral illite pore, an illite pore fully packed with Type II-D kerogen, and a wider illite pore partially filled with kerogen. Under reservoir conditions, supercritical CO₂ was injected into each system, followed by a simulated leakage event. The findings reveal that, although pores with greater void volume store more CO₂ initially, their ability to retain it under leakage conditions is markedly lower. In contrast, kerogen-rich systems retain a significantly larger fraction of the adsorbed CO₂, especially in regions where kerogen is in direct contact with mineral surfaces. These results highlight the critical importance of organic content and mineral–organic interfacial structure in controlling CO₂ retention, offering molecular-level insights into the design of more secure geological storage systems.
{"title":"Molecular insights into the role of kerogen in retention of geologically sequestered CO₂ in shale formations during leakage scenarios","authors":"Zikir A. Kemala , Manav Kakkanat , Andrey G. Kalinichev , Narasimhan Loganathan , Juliana Zaini , Malik M. Nauman , A. Ozgur Yazaydin","doi":"10.1016/j.ccst.2025.100524","DOIUrl":"10.1016/j.ccst.2025.100524","url":null,"abstract":"<div><div>The long-term security of geological CO₂ storage depends not only on the capacity of reservoir rocks to accommodate CO₂ but also on their ability to retain it under leakage scenarios. In this study, molecular dynamics simulations were used to investigate CO₂ behavior in illite-based shale pores with varying organic content and structural configurations. Three representative pore models were examined: a purely mineral illite pore, an illite pore fully packed with Type II-D kerogen, and a wider illite pore partially filled with kerogen. Under reservoir conditions, supercritical CO₂ was injected into each system, followed by a simulated leakage event. The findings reveal that, although pores with greater void volume store more CO₂ initially, their ability to retain it under leakage conditions is markedly lower. In contrast, kerogen-rich systems retain a significantly larger fraction of the adsorbed CO₂, especially in regions where kerogen is in direct contact with mineral surfaces. These results highlight the critical importance of organic content and mineral–organic interfacial structure in controlling CO₂ retention, offering molecular-level insights into the design of more secure geological storage systems.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100524"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217016","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 : 2025-12-01Epub Date: 2025-09-11DOI: 10.1016/j.ccst.2025.100517
Shashank Singh Rawat, Frederico Gomes Fonseca, María Isabel Roldán Serrano
Achieving global net-zero emissions requires widespread adoption of Carbon Capture Utilization and Storage (CCUS) technologies. However, the current state-of-the-art using amines relies on fossil fuel-based thermal energy for solvent regeneration, offsetting some emission reductions. This study proposes and validates an economically viable decarbonization strategy for carbon capture units. The carbon capture unit is evaluated in isolation, proposing different cases focused on varying levels of decarbonization. The methodology utilizes available process waste heat while reducing dependence on external heat supply. A techno-economic evaluation against the background of Germany, considering both the high electricity-fuel price ratio and fossil-heavy electrical supply to be important deterrents. Using Aspen Plus™, an industrial pilot CC unit was simulated, and a conventional High Temperature Heat Pump (HTHP) solution employing hydrocarbons was integrated, reducing external heat demand by 27 % with minor process modifications. More complex integration systems can achieve total decarbonization of the heat supply, albeit at higher costs. The study also investigates the role of carbon credits as both a cost and revenue source, along with sensitivity analyses on process costs and emissions. The present work introduces a novel approach for economic decarbonization of solvent-based carbon capture units. Minor modifications to the operating pressure in the regeneration column were found to increase heat demand and emissions, but also permitted the use of novel HTHP technologies, resulting in even lower process costs and emissions at high electrification levels. The results offer valuable insights for researchers, technology providers, and policymakers seeking to reduce emissions from emission-intensive industries.
{"title":"Innovative high temperature heat pump concepts for an economic decarbonization of a carbon capture unit","authors":"Shashank Singh Rawat, Frederico Gomes Fonseca, María Isabel Roldán Serrano","doi":"10.1016/j.ccst.2025.100517","DOIUrl":"10.1016/j.ccst.2025.100517","url":null,"abstract":"<div><div>Achieving global net-zero emissions requires widespread adoption of Carbon Capture Utilization and Storage (CCUS) technologies. However, the current state-of-the-art using amines relies on fossil fuel-based thermal energy for solvent regeneration, offsetting some emission reductions. This study proposes and validates an economically viable decarbonization strategy for carbon capture units. The carbon capture unit is evaluated in isolation, proposing different cases focused on varying levels of decarbonization. The methodology utilizes available process waste heat while reducing dependence on external heat supply. A techno-economic evaluation against the background of Germany, considering both the high electricity-fuel price ratio and fossil-heavy electrical supply to be important deterrents. Using Aspen Plus™, an industrial pilot CC unit was simulated, and a conventional High Temperature Heat Pump (HTHP) solution employing hydrocarbons was integrated, reducing external heat demand by 27 % with minor process modifications. More complex integration systems can achieve total decarbonization of the heat supply, albeit at higher costs. The study also investigates the role of carbon credits as both a cost and revenue source, along with sensitivity analyses on process costs and emissions. The present work introduces a novel approach for economic decarbonization of solvent-based carbon capture units. Minor modifications to the operating pressure in the regeneration column were found to increase heat demand and emissions, but also permitted the use of novel HTHP technologies, resulting in even lower process costs and emissions at high electrification levels. The results offer valuable insights for researchers, technology providers, and policymakers seeking to reduce emissions from emission-intensive industries.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100517"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217017","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 : 2025-12-01Epub Date: 2025-09-11DOI: 10.1016/j.ccst.2025.100520
Hao Wang , Lei Liu , Hanzi Liu , Xuancan Zhu , Zhiqiang Sun
Integrated CO2 capture and utilization (ICCU) coupled with the reverse water-gas shift reaction offers a promising route to convert captured CO2 into value-added CO using Ca-based dual functional materials (DFMs), providing an economically viable strategy for reducing CO2 emissions from energy and industry sources. However, existing Ca-based DMFs typically require a high H2/CO2 ratio to achieve efficient catalytic CO generation from adsorbed CO2. To address this limitation, this study develops a series of Ni and Ce co-modified Fe-Mn-Ca DFMs that enable high CO2 conversion and CO yield under near-equimolar H2/CO2 conditions in a fixed-bed reactor. Results indicate that CaO modified with a Fe/Mn molar ratio of 7:3 exhibits a CO2 capture capacity of 11.42 mmol g−1 and subsequent CO2 conversion of 58.7 %. Further modification of this optimized Fe-Mn-Ca material with Ni and Ce cooperative enhancement performance, achieving 61 % CO2 conversion and 100 % CO selectivity at a H2/CO2 ratio of 1:1, with only 18 % decay over 10 consecutive cycles. Mechanistic insights into the cyclic CO2 adsorption and hydrogenation processes, as well as performance attenuation, were elucidated through material characterization. The effective formation of formate intermediates is responsible for the production of CO from the adsorbed CO2 under near-equimolar H2/CO2 conditions. Finally, comparative performance analysis and enhancement mechanisms are discussed. These findings establish a material foundation for ICCU systems targeting CO production in a serial dual-fluidized bed reactor.
{"title":"Cooperative enhancement of Ni/Ce-Fe-Mn-Ca dual functional materials for integrated CO2 capture and conversion to CO under near-equimolar H2/CO2 conditions","authors":"Hao Wang , Lei Liu , Hanzi Liu , Xuancan Zhu , Zhiqiang Sun","doi":"10.1016/j.ccst.2025.100520","DOIUrl":"10.1016/j.ccst.2025.100520","url":null,"abstract":"<div><div>Integrated CO<sub>2</sub> capture and utilization (ICCU) coupled with the reverse water-gas shift reaction offers a promising route to convert captured CO<sub>2</sub> into value-added CO using Ca-based dual functional materials (DFMs), providing an economically viable strategy for reducing CO<sub>2</sub> emissions from energy and industry sources. However, existing Ca-based DMFs typically require a high H<sub>2</sub>/CO<sub>2</sub> ratio to achieve efficient catalytic CO generation from adsorbed CO<sub>2</sub>. To address this limitation, this study develops a series of Ni and Ce co-modified Fe-Mn-Ca DFMs that enable high CO<sub>2</sub> conversion and CO yield under near-equimolar H<sub>2</sub>/CO<sub>2</sub> conditions in a fixed-bed reactor. Results indicate that CaO modified with a Fe/Mn molar ratio of 7:3 exhibits a CO<sub>2</sub> capture capacity of 11.42 mmol <em>g</em><sup>−1</sup> and subsequent CO<sub>2</sub> conversion of 58.7 %. Further modification of this optimized Fe-Mn-Ca material with Ni and Ce cooperative enhancement performance, achieving 61 % CO<sub>2</sub> conversion and 100 % CO selectivity at a H<sub>2</sub>/CO<sub>2</sub> ratio of 1:1, with only 18 % decay over 10 consecutive cycles. Mechanistic insights into the cyclic CO<sub>2</sub> adsorption and hydrogenation processes, as well as performance attenuation, were elucidated through material characterization. The effective formation of formate intermediates is responsible for the production of CO from the adsorbed CO<sub>2</sub> under near-equimolar H<sub>2</sub>/CO<sub>2</sub> conditions. Finally, comparative performance analysis and enhancement mechanisms are discussed. These findings establish a material foundation for ICCU systems targeting CO production in a serial dual-fluidized bed reactor.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100520"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096339","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}
Integrated carbon capture and utilisation (ICCU) is a promising technology to mitigate the impact of carbon emissions, as it combines sorbent regeneration and CO2 utilisation. ICCU has been intensively studied for reverse water shift reaction (RWGS), methanation and dry methane reforming (DRM). However, ICCU-RWGS and ICCU-Methanation rely on hydrogen, which compromises economic viability and safety, and the complex synthesis of DFMs for ICCU-DRM, requiring promoters or multilayer structures. To enhance the practicality of ICCU technology, here we investigated carbon-based ICCU (C-ICCU), which utilises the reverse Boudouard reaction with carbon as the reducing agent. In this study, we explored the key operational factors influencing C-ICCU performance, specifically Ni loading, the Ni/graphite mass, and temperature. Our findings indicate that Ni/graphite is a highly effective catalyst for the in-situ conversion of CO2 to CO. Specifically, a Ni loading of 3 wt.% or higher achieved a CO2 conversion greater than 95% at 650°C. Furthermore, in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis revealed the synergistic interactions between graphite and nickel. Specifically, graphite promotes CO2 generation while nickel catalyses its subsequent conversion. Our research demonstrates that the C-ICCU mechanism is a complex synergistic process involving the dynamic evolution of surface species. This work offers a promising, safer, and potentially more economical pathway for industrial carbon capture and utilisation.
{"title":"Graphite–Ni synergy unlocks a hydrogen-free pathway for carbon based integrated CO₂ capture and utilisation (ICCU)","authors":"Junhan Lu, Xiaotong Zhao, Jia Hu, Bo Zong, Yuanyuan Wang, Chunfei Wu","doi":"10.1016/j.ccst.2025.100546","DOIUrl":"10.1016/j.ccst.2025.100546","url":null,"abstract":"<div><div>Integrated carbon capture and utilisation (ICCU) is a promising technology to mitigate the impact of carbon emissions, as it combines sorbent regeneration and CO<sub>2</sub> utilisation. ICCU has been intensively studied for reverse water shift reaction (RWGS), methanation and dry methane reforming (DRM). However, ICCU-RWGS and ICCU-Methanation rely on hydrogen, which compromises economic viability and safety, and the complex synthesis of DFMs for ICCU-DRM, requiring promoters or multilayer structures. To enhance the practicality of ICCU technology, here we investigated carbon-based ICCU (C-ICCU), which utilises the reverse Boudouard reaction with carbon as the reducing agent. In this study, we explored the key operational factors influencing C-ICCU performance, specifically Ni loading, the Ni/graphite mass, and temperature. Our findings indicate that Ni/graphite is a highly effective catalyst for the in-situ conversion of CO<sub>2</sub> to CO. Specifically, a Ni loading of 3 wt.% or higher achieved a CO<sub>2</sub> conversion greater than 95% at 650°C. Furthermore, in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis revealed the synergistic interactions between graphite and nickel. Specifically, graphite promotes CO<sub>2</sub> generation while nickel catalyses its subsequent conversion. Our research demonstrates that the C-ICCU mechanism is a complex synergistic process involving the dynamic evolution of surface species. This work offers a promising, safer, and potentially more economical pathway for industrial carbon capture and utilisation.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100546"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145680891","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 : 2025-12-01Epub Date: 2025-10-08DOI: 10.1016/j.ccst.2025.100530
Lun Wang , Yuhang Liu , Zhanhai Li , Xilin Gu , Lijun Yu
The growing deployment of renewable energy sources (RES) often leads to large-scale curtailment. Direct air capture (DAC) systems—energy-intensive yet dispatchable and modular—offer a promising solution for consuming curtailment while enabling negative emissions. However, the integration of DAC with RES remains underexplored. Specifically, DAC systems lack sufficient flexibility to accommodate intermittent energy supplies, stemming from inadequate temporal resolution of operational strategies and overly rigid operational assumptions. Moreover, their operation relies on historical data, lacking real-time control and coordinated scheduling with power plants. To bridge this gap, this study proposes a multi-timescale optimization scheduling framework that enables minute-level real-time control of modular DAC systems co-located with RES power plants. The approach uniquely integrates transferable and curtailable flexible operation modes within a two-phase scheduling system—combining day-ahead planning with intraday rolling optimization—while incorporating power forecast data from RES plants to eliminate perfect-foresight assumptions inherent in retrospective optimization, thereby establishing the first implementable real-time controlled co-dispatch architecture for synergistic RES-DAC integration. A case study based on real-world data from an 850 MW wind farm demonstrates that this approach can reduce daily system operation costs by a factor of five, increase the utilization rate of curtailed electricity to over 90%, and capture 1.5 million tons of CO2 annually. Collectively, these outcomes establish an effective scheduling solution for RES-DAC integration that simultaneously enhances environmental sustainability and economic returns.
{"title":"Research on the multi-timescale optimization scheduling of direct air capture systems driven by renewable energy","authors":"Lun Wang , Yuhang Liu , Zhanhai Li , Xilin Gu , Lijun Yu","doi":"10.1016/j.ccst.2025.100530","DOIUrl":"10.1016/j.ccst.2025.100530","url":null,"abstract":"<div><div>The growing deployment of renewable energy sources (RES) often leads to large-scale curtailment. Direct air capture (DAC) systems—energy-intensive yet dispatchable and modular—offer a promising solution for consuming curtailment while enabling negative emissions. However, the integration of DAC with RES remains underexplored. Specifically, DAC systems lack sufficient flexibility to accommodate intermittent energy supplies, stemming from inadequate temporal resolution of operational strategies and overly rigid operational assumptions. Moreover, their operation relies on historical data, lacking real-time control and coordinated scheduling with power plants. To bridge this gap, this study proposes a multi-timescale optimization scheduling framework that enables minute-level real-time control of modular DAC systems co-located with RES power plants. The approach uniquely integrates transferable and curtailable flexible operation modes within a two-phase scheduling system—combining day-ahead planning with intraday rolling optimization—while incorporating power forecast data from RES plants to eliminate perfect-foresight assumptions inherent in retrospective optimization, thereby establishing the first implementable real-time controlled co-dispatch architecture for synergistic RES-DAC integration. A case study based on real-world data from an 850 MW wind farm demonstrates that this approach can reduce daily system operation costs by a factor of five, increase the utilization rate of curtailed electricity to over 90%, and capture 1.5 million tons of CO<sub>2</sub> annually. Collectively, these outcomes establish an effective scheduling solution for RES-DAC integration that simultaneously enhances environmental sustainability and economic returns.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100530"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145320915","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 : 2025-12-01Epub 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":"2025-12-01","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}
Pub Date : 2025-12-01Epub Date: 2025-10-24DOI: 10.1016/j.ccst.2025.100534
Jia Song , Long Shi , Jing Wei , Min Deng , Zikang Qin , Lin Yang , Junfeng Zheng , Wenju Jiang , Lu Yao , Zhongde Dai
Axial coordination engineering is a promising method to regulate the active sites of single atom catalysts (SACs) in electrochemical reduction of CO2 (ECR) and further realize the manipulating of the electrocatalytic activity, selectivity, and stability of catalysts. Here, a facile post-synthetic modification strategy of metal exchange and heteroatom dopant was proposed to develop a single iron atom catalyst coordinated with four planar N atoms and one axial Br atom (denoted as Fex-NCBry) for ECR to CO. By altering the operating conditions including pyrolysis temperature as well as dopant amount of Fe and Br, the optimized Fe20-NCBr0.3 catalyst acquired more surface-active sites and lower impedance, exhibiting an enhanced CO selectivity of 93.78 % with a CO reduction current density of -21.16 mA cm-2 at -0.9 V (vs. RHE). This work provides new possibilities for tuning the SACs coordination environment with an axial heteroatom for improved ECR performance.
轴向配位工程是调控电化学还原CO2过程中单原子催化剂活性位点,进而实现对催化剂电催化活性、选择性和稳定性的调控的一种很有前景的方法。本文提出了一种简单的金属交换和杂原子掺杂的合成后改性策略,开发了一种单铁原子与四个平面N原子和一个轴向Br原子(Fex-NCBry)配位的ECR - CO催化剂。通过改变热解温度、Fe和Br的掺杂量等操作条件,优化后的Fe20-NCBr0.3催化剂获得了更多的表面活性位点和更低的阻抗。在-0.9 V(相对于RHE)下,CO还原电流密度为-21.16 mA cm-2时,CO选择性提高了93.78%。这项工作为通过轴向杂原子调整SACs配位环境以提高ECR性能提供了新的可能性。
{"title":"Enhancing CO2 electroreduction over iron-nitrogen-doped carbon catalysts by axial bromine coordination","authors":"Jia Song , Long Shi , Jing Wei , Min Deng , Zikang Qin , Lin Yang , Junfeng Zheng , Wenju Jiang , Lu Yao , Zhongde Dai","doi":"10.1016/j.ccst.2025.100534","DOIUrl":"10.1016/j.ccst.2025.100534","url":null,"abstract":"<div><div>Axial coordination engineering is a promising method to regulate the active sites of single atom catalysts (SACs) in electrochemical reduction of CO<sub>2</sub> (ECR) and further realize the manipulating of the electrocatalytic activity, selectivity, and stability of catalysts. Here, a facile post-synthetic modification strategy of metal exchange and heteroatom dopant was proposed to develop a single iron atom catalyst coordinated with four planar N atoms and one axial Br atom (denoted as Fe<sub>x</sub><sub>-</sub>NCBr<sub>y</sub>) for ECR to CO. By altering the operating conditions including pyrolysis temperature as well as dopant amount of Fe and Br, the optimized Fe<sub>20</sub>-NCBr<sub>0.3</sub> catalyst acquired more surface-active sites and lower impedance, exhibiting an enhanced CO selectivity of 93.78 % with a CO reduction current density of -21.16 mA cm<sup>-</sup><sup>2</sup> at -0.9 V (vs. RHE). This work provides new possibilities for tuning the SACs coordination environment with an axial heteroatom for improved ECR performance.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100534"},"PeriodicalIF":0.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145412814","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}