Pub 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":"2025-09-26","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 : 2025-09-22DOI: 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":"2025-09-22","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 : 2025-09-22DOI: 10.1016/j.ccst.2025.100523
Kayode Adesina Adegoke, Potlaki Foster Tseki
The CO2 reduction reactions present a viable approach to addressing the challenges of energy scarcity and the pressing concerns of global warming. To enhance their kinetically sluggish processes, developing highly stable, cost-effective, selective, and energy-efficient catalysts is essential. Graphene-based metal-organic frameworks (MOFs) composite exhibits characteristics such as outstanding conductivity, structural tunability, and excellent surface chemistry and sustainability, positioning them as innovative competitors for both CO2 conversion to fuels and chemicals. In this study, we present recent developments in graphene-based MOF catalysts for CO2 reduction reactions (CO2RR). Before discussing the evaluation of the approaches for graphene-based MOFs, rational, structural, and electronic synergies of graphene/MOF nanocomposites were addressed. Various synthetic techniques, a comprehensive review of characterization techniques, associated challenges, and the relation between graphene-based MOF structures and their conductivity are examined. A detailed breakthrough in both photocatalytic and electrocatalytic performance for CO2RR is examined. The concluding remarks emphasized the knowledge gaps, related deficiencies, and strengths, with significant viewpoints and concepts for enhancing graphene-based MOFs for CO2RR in accordance with pragmatic industry expectations. This study offers the scientific community a thorough insight into the present research emphasis and the significance of creating more efficient and environmentally sustainable graphene-based MOFs for clean energy conversion. This is essential for tackling the difficulties of reducing greenhouse gas emissions and alleviating the global energy deficit.
{"title":"Graphene-based metal-organic framework nanocomposites for CO2 reduction reactions","authors":"Kayode Adesina Adegoke, Potlaki Foster Tseki","doi":"10.1016/j.ccst.2025.100523","DOIUrl":"10.1016/j.ccst.2025.100523","url":null,"abstract":"<div><div>The CO<sub>2</sub> reduction reactions present a viable approach to addressing the challenges of energy scarcity and the pressing concerns of global warming. To enhance their kinetically sluggish processes, developing highly stable, cost-effective, selective, and energy-efficient catalysts is essential. Graphene-based metal-organic frameworks (MOFs) composite exhibits characteristics such as outstanding conductivity, structural tunability, and excellent surface chemistry and sustainability, positioning them as innovative competitors for both CO<sub>2</sub> conversion to fuels and chemicals. In this study, we present recent developments in graphene-based MOF catalysts for CO<sub>2</sub> reduction reactions (CO<sub>2</sub>RR). Before discussing the evaluation of the approaches for graphene-based MOFs, rational, structural, and electronic synergies of graphene/MOF nanocomposites were addressed. Various synthetic techniques, a comprehensive review of characterization techniques, associated challenges, and the relation between graphene-based MOF structures and their conductivity are examined. A detailed breakthrough in both photocatalytic and electrocatalytic performance for CO<sub>2</sub>RR is examined. The concluding remarks emphasized the knowledge gaps, related deficiencies, and strengths, with significant viewpoints and concepts for enhancing graphene-based MOFs for CO<sub>2</sub>RR in accordance with pragmatic industry expectations. This study offers the scientific community a thorough insight into the present research emphasis and the significance of creating more efficient and environmentally sustainable graphene-based MOFs for clean energy conversion. This is essential for tackling the difficulties of reducing greenhouse gas emissions and alleviating the global energy deficit.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100523"},"PeriodicalIF":0.0,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145320913","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 : 2025-09-16DOI: 10.1016/j.ccst.2025.100516
Milad Shakouri Kalfati, Ahmed Abdulla
Averting the worst consequences of climate change requires decarbonizing the global energy system and deploying carbon dioxide removal technologies, including the direct air capture of CO. To estimate the cost and performance of the latter technologies, climate and energy system analysts need numerical process models that are validated with experimental data. Existing process models often limit reconfiguration that accommodates different design choices or restrict modelling to steady-state conditions. However, ambient environmental conditions like temperature, humidity, pressure, and inlet CO concentration vary, affecting capture. This study develops an open-source process model for direct air capture using solid sorbents. Starting from first principles, this model allows users to select facility sizes, sorbents, other design parameters, and locations to simulate the capture performance of a solid sorbent direct air capture plant. More importantly, users can incorporate climate data to determine site-specific performance. Here, model validation is presented for two cold-climate sorbents that are being proposed for nations in northern latitudes. Results for climatically different cities are presented, highlighting the importance of sorbent choice and ambient environmental conditions on the overall capture performance and energy requirement of a direct air capture facility. The model can be employed by engineers, investors, and energy system analysts to undertake design optimization research, siting analyses, and improved studies that integrate high-fidelity process models into energy system optimization.
{"title":"An open-source dynamic model for direct air capture of carbon dioxide using solid sorbents","authors":"Milad Shakouri Kalfati, Ahmed Abdulla","doi":"10.1016/j.ccst.2025.100516","DOIUrl":"10.1016/j.ccst.2025.100516","url":null,"abstract":"<div><div>Averting the worst consequences of climate change requires decarbonizing the global energy system and deploying carbon dioxide removal technologies, including the direct air capture of CO<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span>. To estimate the cost and performance of the latter technologies, climate and energy system analysts need numerical process models that are validated with experimental data. Existing process models often limit reconfiguration that accommodates different design choices or restrict modelling to steady-state conditions. However, ambient environmental conditions like temperature, humidity, pressure, and inlet CO<span><math><msub><mrow></mrow><mn>2</mn></msub></math></span> concentration vary, affecting capture. This study develops an open-source process model for direct air capture using solid sorbents. Starting from first principles, this model allows users to select facility sizes, sorbents, other design parameters, and locations to simulate the capture performance of a solid sorbent direct air capture plant. More importantly, users can incorporate climate data to determine site-specific performance. Here, model validation is presented for two cold-climate sorbents that are being proposed for nations in northern latitudes. Results for climatically different cities are presented, highlighting the importance of sorbent choice and ambient environmental conditions on the overall capture performance and energy requirement of a direct air capture facility. The model can be employed by engineers, investors, and energy system analysts to undertake design optimization research, siting analyses, and improved studies that integrate high-fidelity process models into energy system optimization.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100516"},"PeriodicalIF":0.0,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145262668","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 : 2025-09-16DOI: 10.1016/j.ccst.2025.100521
Hafiz Muhammad Waqar Abid , Mannix P. Balanay
The electrochemical reduction of carbon dioxide (CO2RR) represents a promising pathway toward sustainable and carbon-neutral production of fuels and chemicals. Among various electrocatalysts, copper-based metal–organic frameworks (Cu-MOFs) have emerged as a highly versatile class of materials. This review provides a comprehensive overview of Cu-MOF-based electrocatalysts, with a particular focus on controlling rate and product selectivity toward C1 (CO, HCOOH, CH4, CH3OH) and C2 (C2H4, C2H5OH) compounds. We critically examine how operando/DFT informed factors such as metal-ligand coordination, framework topology, and electronic structure influence key mechanistic steps of CO2RR. Persistent challenges such as low intrinsic electrical conductivity, structural instability, and insufficient selectivity toward multicarbon products are thoroughly examined. This review is distinctive in connecting fundamental mechanistic pathways of CO2RR with material design, highlighting how π-conjugated linkers, heteroatom doping, in situ reconstruction and derivatives, as well as hydrophobic surface engineering can be harnessed to optimize activity, selectivity and stability. Particular attention is given to operando and in situ characterization techniques. Finally, we propose a future roadmap that integrates band structure engineering, development of bimetallic and multi-functional active sites, and implementation of standardized testing protocols. By bridging mechanistic understanding with rational material design, this review aims to accelerate the development of high-performance, durable, and scalable Cu-MOF-based electrocatalysts for efficient CO₂ reduction.
{"title":"Next-Generation Cu-MOF-based electrocatalysts for CO2 reduction: Bridging mechanistic insights and rational design","authors":"Hafiz Muhammad Waqar Abid , Mannix P. Balanay","doi":"10.1016/j.ccst.2025.100521","DOIUrl":"10.1016/j.ccst.2025.100521","url":null,"abstract":"<div><div>The electrochemical reduction of carbon dioxide (CO<sub>2</sub>RR) represents a promising pathway toward sustainable and carbon-neutral production of fuels and chemicals. Among various electrocatalysts, copper-based metal–organic frameworks (Cu-MOFs) have emerged as a highly versatile class of materials. This review provides a comprehensive overview of Cu-MOF-based electrocatalysts, with a particular focus on controlling rate and product selectivity toward C<sub>1</sub> (CO, HCOOH, CH<sub>4</sub>, CH<sub>3</sub>OH) and C<sub>2</sub> (C<sub>2</sub>H<sub>4</sub>, C<sub>2</sub>H<sub>5</sub>OH) compounds. We critically examine how operando/DFT informed factors such as metal-ligand coordination, framework topology, and electronic structure influence key mechanistic steps of CO<sub>2</sub>RR. Persistent challenges such as low intrinsic electrical conductivity, structural instability, and insufficient selectivity toward multicarbon products are thoroughly examined. This review is distinctive in connecting fundamental mechanistic pathways of CO<sub>2</sub>RR with material design, highlighting how π-conjugated linkers, heteroatom doping, in situ reconstruction and derivatives, as well as hydrophobic surface engineering can be harnessed to optimize activity, selectivity and stability. Particular attention is given to operando and in situ characterization techniques. Finally, we propose a future roadmap that integrates band structure engineering, development of bimetallic and multi-functional active sites, and implementation of standardized testing protocols. By bridging mechanistic understanding with rational material design, this review aims to accelerate the development of high-performance, durable, and scalable Cu-MOF-based electrocatalysts for efficient CO₂ reduction.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100521"},"PeriodicalIF":0.0,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145155274","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 : 2025-09-11DOI: 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":"2025-09-11","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 : 2025-09-11DOI: 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":"2025-09-11","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}
Pub Date : 2025-09-11DOI: 10.1016/j.ccst.2025.100519
Qingqin Wang, Zichen Cao, Qingqing Li, Bing Song
The escalating atmospheric CO2 concentration and concomitant ecological crises underscore the urgent need for innovative carbon capture and utilization strategies. Fly ash (FA), a global industrial byproduct with annual production exceeding 1 billion tons, presents a promising opportunity for simultaneous CO2 mineralization and heavy metal stabilization. This review systematically examines recent advancements in FA-mediated CO2 sequestration coupled with heavy metal immobilization, addressing critical knowledge gaps in their synergistic mechanisms. We analyze the interplay between carbonation pathways and heavy metal fate, the effects of key reaction parameters on Ca2+ leaching efficiency and metal stabilization, and the impact of pre-treatment methods such as mechanical activation and acid/alkali modification. Furthermore, we review the application of theoretical calculations for atomic-scale mechanism analysis and process optimization via machine learning. Finally, we identify existing challenges—including kinetic limitations, pH-dependent metal mobilization, and economic viability—and propose future research directions for enhancing process efficiency and environmental safety. This review aims to facilitate the development of fly ash-based technologies for dual carbon sequestration and pollution control, contributing to sustainable industrial solid waste management.
{"title":"Advances in concurrent CO2 sequestration and heavy metal mobilization during fly ash carbonation: A review","authors":"Qingqin Wang, Zichen Cao, Qingqing Li, Bing Song","doi":"10.1016/j.ccst.2025.100519","DOIUrl":"10.1016/j.ccst.2025.100519","url":null,"abstract":"<div><div>The escalating atmospheric CO<sub>2</sub> concentration and concomitant ecological crises underscore the urgent need for innovative carbon capture and utilization strategies. Fly ash (FA), a global industrial byproduct with annual production exceeding 1 billion tons, presents a promising opportunity for simultaneous CO<sub>2</sub> mineralization and heavy metal stabilization. This review systematically examines recent advancements in FA-mediated CO<sub>2</sub> sequestration coupled with heavy metal immobilization, addressing critical knowledge gaps in their synergistic mechanisms. We analyze the interplay between carbonation pathways and heavy metal fate, the effects of key reaction parameters on Ca<sup>2+</sup> leaching efficiency and metal stabilization, and the impact of pre-treatment methods such as mechanical activation and acid/alkali modification. Furthermore, we review the application of theoretical calculations for atomic-scale mechanism analysis and process optimization via machine learning. Finally, we identify existing challenges—including kinetic limitations, pH-dependent metal mobilization, and economic viability—and propose future research directions for enhancing process efficiency and environmental safety. This review aims to facilitate the development of fly ash-based technologies for dual carbon sequestration and pollution control, contributing to sustainable industrial solid waste management.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100519"},"PeriodicalIF":0.0,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096336","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 : 2025-09-08DOI: 10.1016/j.ccst.2025.100509
Robert Kiefel , Jonas Görtz , Jan Haß , Julius Walorski , Falk Zimmer , Andreas Jupke
<div><div>The industrial deployment of <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> capture technologies for purifying gases with low <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> partial pressure (e.g., flue gas) has been limited due to substantial economic hurdles. Process intensification offers a pathway to enhance the cost efficiency of <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> sequestration. One approach that has garnered significant attention is the process integration of phase-change absorbents. Among these, bis(iminoguanidines) have shown considerable promise in recent literature. Particularly, glyoxal-bis(iminoguanidine) (GBIG) has demonstrated the ability to precipitate <span><math><msubsup><mrow><mi>HCO</mi></mrow><mrow><mn>3</mn></mrow><mo>−</mo></msubsup></math></span> with low regeneration energy demand. However, GBIG and comparable phase-change absorbents require the integration of alkaline scrubbing with reactive precipitation in a single unit operation (gas-liquid reactive precipitation), introducing operational challenges such as scaling and clogging in conventionally applied packed-bed columns. To mitigate these issues, this study investigates the use of a spray tower as a gas-liquid reactive precipitator for <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> capture from a flue gas surrogate. A pilot-scale spray tower is designed, constructed, and operated. Contrary to expectations, Rayleigh breakup of liquid jets induces a bimodal droplet size distribution in the lower sections of the tower, indicating limited scalability and highlighting the need for liquid recycling. For comparative purposes, the investigation includes a <span><math><msubsup><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mrow><mn>3</mn></mrow><mrow><mn>2</mn><mo>−</mo></mrow></msubsup></math></span>-precipitating system (<span><math><msub><mrow><mi>Ba</mi><mo>(</mo><mtext>OH</mtext><mo>)</mo></mrow><mn>2</mn></msub></math></span>) and a non-precipitating system (<span><math><mrow><mi>NaOH</mi></mrow></math></span>), alongside GBIG. All systems demonstrate stable operability in single-pass and batch modes. During liquid recycling, small amounts of solids are entrained to the tower top. Nevertheless, no evidence of scaling or clogging is detected at the orifice plate, suggesting that the precipitated solids are significantly smaller than the orifice diameter. In the final performance comparison, the <span><math><mrow><mi>GBIG</mi></mrow></math></span> system demonstrates superior <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> capture efficiency relative to the <span><math><msub><mrow><mi>Ba</mi><mo>(</mo><mtext>OH</mtext><mo>)</mo></mrow><mn>2</mn></msub></math></span> system. However, achieving this efficiency com
{"title":"Feasibility assessment of a spray tower for gas-liquid reactive precipitation in CO2 capture","authors":"Robert Kiefel , Jonas Görtz , Jan Haß , Julius Walorski , Falk Zimmer , Andreas Jupke","doi":"10.1016/j.ccst.2025.100509","DOIUrl":"10.1016/j.ccst.2025.100509","url":null,"abstract":"<div><div>The industrial deployment of <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> capture technologies for purifying gases with low <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> partial pressure (e.g., flue gas) has been limited due to substantial economic hurdles. Process intensification offers a pathway to enhance the cost efficiency of <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> sequestration. One approach that has garnered significant attention is the process integration of phase-change absorbents. Among these, bis(iminoguanidines) have shown considerable promise in recent literature. Particularly, glyoxal-bis(iminoguanidine) (GBIG) has demonstrated the ability to precipitate <span><math><msubsup><mrow><mi>HCO</mi></mrow><mrow><mn>3</mn></mrow><mo>−</mo></msubsup></math></span> with low regeneration energy demand. However, GBIG and comparable phase-change absorbents require the integration of alkaline scrubbing with reactive precipitation in a single unit operation (gas-liquid reactive precipitation), introducing operational challenges such as scaling and clogging in conventionally applied packed-bed columns. To mitigate these issues, this study investigates the use of a spray tower as a gas-liquid reactive precipitator for <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> capture from a flue gas surrogate. A pilot-scale spray tower is designed, constructed, and operated. Contrary to expectations, Rayleigh breakup of liquid jets induces a bimodal droplet size distribution in the lower sections of the tower, indicating limited scalability and highlighting the need for liquid recycling. For comparative purposes, the investigation includes a <span><math><msubsup><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mrow><mn>3</mn></mrow><mrow><mn>2</mn><mo>−</mo></mrow></msubsup></math></span>-precipitating system (<span><math><msub><mrow><mi>Ba</mi><mo>(</mo><mtext>OH</mtext><mo>)</mo></mrow><mn>2</mn></msub></math></span>) and a non-precipitating system (<span><math><mrow><mi>NaOH</mi></mrow></math></span>), alongside GBIG. All systems demonstrate stable operability in single-pass and batch modes. During liquid recycling, small amounts of solids are entrained to the tower top. Nevertheless, no evidence of scaling or clogging is detected at the orifice plate, suggesting that the precipitated solids are significantly smaller than the orifice diameter. In the final performance comparison, the <span><math><mrow><mi>GBIG</mi></mrow></math></span> system demonstrates superior <span><math><msub><mrow><mrow><mi>C</mi></mrow><mi>O</mi></mrow><mn>2</mn></msub></math></span> capture efficiency relative to the <span><math><msub><mrow><mi>Ba</mi><mo>(</mo><mtext>OH</mtext><mo>)</mo></mrow><mn>2</mn></msub></math></span> system. However, achieving this efficiency com","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100509"},"PeriodicalIF":0.0,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096340","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 : 2025-09-07DOI: 10.1016/j.ccst.2025.100518
Paul de Joannis , Christophe Castel , Mohamed Kanniche , Eric Favre , Olivier Authier
This study investigates a direct air capture (DAC) process using a solid-DAC S-VTSA (steam-assisted vacuum thermal swing adsorption) process. A commercially available sorbent, commonly used in packed bed configurations, is selected as the benchmark sorbent, while a monolithic geometry is also examined to assess its potential performance. The process is modelled using Aspen Adsorption and incorporates physico-chemical data in DAC environmental conditions, including binary isotherms under humid condition. In a reference case comparing the two geometries, the packed bed exhibits higher productivity (2.4 kgCO2/(h.m3)), while the monolith achieves 1.2 kgCO2/(h.m3). However, the monolith allows for a significant reduction in pressure drop and associated fan work by about two orders of magnitude. These findings highlight the trade-off between productivity in favor of packed bed and energy requirement in favor of monolithic design. A sensitivity analysis is then conducted on various environmental and process parameters such as sorbent and bed dimension, air velocity, temperature and humidity, adsorption/desorption loading, mass transfer kinetic, and regeneration pressure, temperature, and steam flowrate. Detailed techno-economic analysis, using Aspen Process Economic Analyzer software for capital cost estimation, is performed at capture scale of 100 ktCO2/yr, with capture costs higher than 1500 €/tCO2.
{"title":"Techno-economic analysis of packed bed and structured adsorbent for direct air capture","authors":"Paul de Joannis , Christophe Castel , Mohamed Kanniche , Eric Favre , Olivier Authier","doi":"10.1016/j.ccst.2025.100518","DOIUrl":"10.1016/j.ccst.2025.100518","url":null,"abstract":"<div><div>This study investigates a direct air capture (DAC) process using a solid-DAC S-VTSA (steam-assisted vacuum thermal swing adsorption) process. A commercially available sorbent, commonly used in packed bed configurations, is selected as the benchmark sorbent, while a monolithic geometry is also examined to assess its potential performance. The process is modelled using Aspen Adsorption and incorporates physico-chemical data in DAC environmental conditions, including binary isotherms under humid condition. In a reference case comparing the two geometries, the packed bed exhibits higher productivity (2.4 kgCO<sub>2</sub>/(h.m<sup>3</sup>)), while the monolith achieves 1.2 kgCO<sub>2</sub>/(h.m<sup>3</sup>). However, the monolith allows for a significant reduction in pressure drop and associated fan work by about two orders of magnitude. These findings highlight the trade-off between productivity in favor of packed bed and energy requirement in favor of monolithic design. A sensitivity analysis is then conducted on various environmental and process parameters such as sorbent and bed dimension, air velocity, temperature and humidity, adsorption/desorption loading, mass transfer kinetic, and regeneration pressure, temperature, and steam flowrate. Detailed techno-economic analysis, using Aspen Process Economic Analyzer software for capital cost estimation, is performed at capture scale of 100 ktCO<sub>2</sub>/yr, with capture costs higher than 1500 €/tCO<sub>2</sub>.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100518"},"PeriodicalIF":0.0,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217018","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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