Carbon Capture Science & Technology最新文献

{"title":"Mechanistic elucidation of cascade CO2 hydrogenation enabled by Cu–Fe interfaces and oxygen vacancies","authors":"Hyeonji Yeom,&nbsp;Yongseok Kim,&nbsp;Woosung Leem,&nbsp;Jongmin Park,&nbsp;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 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 C_5–11 hydrocarbons, achieving the highest C_5–11 productivity of 290.7 mL g_cat^–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.</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}

{"title":"Assessing CO2 storage potential in a structurally complex depleted gas reservoir, offshore South Africa","authors":"S. Mhlambi ,&nbsp;O.E. Eruteya ,&nbsp;F.A. Agbor ,&nbsp;A. Moscariello ,&nbsp;J.M. van Bever Donker ,&nbsp;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 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.</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}

{"title":"Optimizing regional CCUS clusterization deployment for multi-industrial sectors: A carbon neutrality pathway for emission-intensive region","authors":"Jianqiao Zhang ,&nbsp;Liang Zhao ,&nbsp;Li Jin ,&nbsp;Chen Zhu ,&nbsp;Haiou Wang ,&nbsp;Lijuan Wang","doi":"10.1016/j.ccst.2025.100495","DOIUrl":"10.1016/j.ccst.2025.100495","url":null,"abstract":"<div><div>Rapid mitigation of global climate change demands transformative technological innovations to achieve deep decarbonization. China has pledged the dual carbon goals of peaking carbon emissions by 2030 and achieving carbon neutrality by 2060, underscoring the urgency and scale of the challenge. While Carbon Capture, Utilization, and Storage (CCUS) has emerged as a promising approach, its large-scale implementation in emission-intensive industrial clustered region faces significant infrastructural challenges. Specifically, the optimal layout of regional CCUS clusterization and CO₂ transport networks remains unclear, particularly in highly industrialized regions such as China’s Jiangsu Province, where diverse industrial sectors and varied geological formations create complex source-sink matching challenges for CCUS deployment. In this study, we developed the SPATIAL (Strategic Pipeline And Technical Integration Analysis Layout) model that enables the optimization of CCUS deployment in emission-intensive regions from an industrial cluster perspective by integrating data of emissions from major industrial sources and storage potential from geological formations. The model was applied to Jiangsu Province under high, medium, and low emission reduction target scenarios through source-sink matching. Results show significant spatial heterogeneity between emission sources and geological storage resources in Jiangsu Province. For example, southern Jiangsu, characterized by high-intensity CO₂ emission clusters, accounts for 63 % of the province’s total emissions while holding only 0.03 % of the province’s geological storage potential. The optimal layout for regional CCUS clusterization deployment under high, medium, and low emission reduction targets achieve total CO₂ storage of 1.4, 1.1, and 0.9 Gt, respectively, supported by pipeline networks of 4629, 2513, and 1433 km. These layouts demonstrate economies of scale, with unit emission reduction costs ranging from 93.84 to 179.31 CNY/t CO₂. Our findings establish the technical and economic feasibility of achieving significant emission reductions through regional CCUS clusterization deployment and address a critical gap in ignoring the hot spot phenomenon of industrial cluster. This study further emphasizes the importance of inter-regional coordination, regional geological storage resource management, and integrated infrastructure planning in realizing cost-effective CCUS clusterization implementation. This study provides policymakers with actionable insights for formulating CCUS clusterization strategies in emission-intensive industrial regions, contributing to the broader goal of regional carbon neutrality.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100495"},"PeriodicalIF":0.0,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145020149","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}

{"title":"Energy-efficient CO2 capture with piperazine and 3-dimethylamino-1-propanol blends: Modeling, experimental validation, and regeneration energy optimization","authors":"Ye-Sub Son ,&nbsp;Shaukat Ali Mazari ,&nbsp;Min-Kyeong Oh ,&nbsp;Gwan Hong Min ,&nbsp;Hyung Jin Park ,&nbsp;Sunghoon Lee ,&nbsp;Il-Hyun Baek ,&nbsp;Chang-Ha Lee ,&nbsp;Jong-Ho Moon ,&nbsp;Sung-Chan Nam","doi":"10.1016/j.ccst.2025.100493","DOIUrl":"10.1016/j.ccst.2025.100493","url":null,"abstract":"<div><div>The contribution of solvent regeneration energy to amine-based CO₂ capture processes is a major hurdle to their large-scale economic viability. It is important to develop solvents that reduce CO₂ capture cost without compromising the process performance or operations. To reduce regeneration energy, this study focuses on the development of aqueous blends of piperazine (PZ) and 3-dimethylamino-1-propanol (3DMA1P) as an energy-efficient absorbent for CO₂ capture. The study relies on rigorous modeling, supported by experimental data. The experimental data from this study and the literature includes CO₂ solubility, NMR speciation, heat of absorption, and physical properties. To determine the potential application of PZ-3DMA1P blend for CO₂ capture, their equilibrium CO₂ solubility, cyclic capacity, heat of absorption, and, more importantly, solvent regeneration energy was investigated. Regeneration energy is calculated and evaluated under the influence of various operating parameters such as absorber temperature (313.15–343.15 K), stripper temperature (373.15–403.15 K), CO₂ partial pressure (1–30 kPa), stripper total pressure (200–400 kPa), CO₂ recovery (80–95 %), amine blending ratio (PZ:3DMA1P, 0–10:40–30 wt.%) and water concentration (60–90 wt.%). The results were compared with those obtained under the same operating conditions using monoethanolamine (MEA) 30 and 40 wt.%, and CESAR-1, the benchmark solvents. Results of the current study for blends of PZ and 3DMA1P are promising, and the solvent system exhibits higher CO₂ absorption capacity and lower regeneration energy compared to MEA and CESAR-1. A comprehensive parametric analysis of regeneration energy enhances the applicability of the results across a diverse range of industries.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100493"},"PeriodicalIF":0.0,"publicationDate":"2025-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144913238","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}

{"title":"Perspectives on the status and future of sustainable CO2 conversion processes and their implementation","authors":"Yakubu Adekunle Alli ,&nbsp;Onome Ejeromedoghene ,&nbsp;Tendai O. Dembaremba ,&nbsp;Amer Adawi ,&nbsp;Oyekunle Azeez Alimi ,&nbsp;Teckla Njei ,&nbsp;Abayomi Bamisaye ,&nbsp;Alex Kofi ,&nbsp;Uche Quincy Anene ,&nbsp;Adekola Monsuru Adewale ,&nbsp;Zainab Temitope Yaqub ,&nbsp;Motunrayo Eniola Oladele ,&nbsp;Lateefat Jimoh ,&nbsp;Samuel Oluwadadepo Oni ,&nbsp;Adeniyi Sunday Ogunlaja ,&nbsp;Ben Bin Xu","doi":"10.1016/j.ccst.2025.100496","DOIUrl":"10.1016/j.ccst.2025.100496","url":null,"abstract":"<div><div>The rapid rise in atmospheric carbon dioxide (CO₂) concentrations continues to threaten global climate stability, underscoring the urgent need for scalable, economically viable, and sustainable CO₂ mitigation strategies. Among emerging solutions, CO₂ conversion technologies offer a transformative pathway by enabling the utilization of CO₂ as a renewable carbon feedstock for the production of fuels, chemicals, and materials, thereby promoting a circular carbon economy. The review begins by exploring foundational CO₂ capture and pre-treatment methods, emphasizing advanced materials, as well as integration strategies that directly couple capture with conversion processes as a gateway to improved CO₂ conversion. Recent advancements in CO₂ conversion technologies, spanning thermochemical, electrochemical, photochemical, and biological domains are then covered. The integration of CO₂ conversion systems with renewable energy and industrial infrastructures is explored through case studies and commercialization efforts, highlighting opportunities for sector-wide decarbonization. Furthermore, the increasing role of artificial intelligence (AI) and machine learning (ML) in predictive modeling, catalyst design, and process optimization, as well as the techno-economic analyses that frame the practical deployment of these technologies is also presented. Persistent challenges including energy efficiency, long-term stability, product selectivity, and regulatory constraints are critically analyzed, and emerging solutions are proposed. The review concludes by outlining future research directions, including the development of next-generation technologies and strategies to promote interdisciplinary collaboration and public-private partnerships. By synthesizing cutting-edge advancements and identifying key barriers and opportunities, this work provides a roadmap for accelerating the global deployment of CO₂ conversion technologies toward a sustainable and decarbonized future.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100496"},"PeriodicalIF":0.0,"publicationDate":"2025-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144913319","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}

{"title":"Artificial Intelligence Prediction of Carbonate Crystallinity of Carbon Mineralization","authors":"Jin Kim ,&nbsp;Seokyoon Moon ,&nbsp;Dongjae Kim","doi":"10.1016/j.ccst.2025.100494","DOIUrl":"10.1016/j.ccst.2025.100494","url":null,"abstract":"<div><div>The importance of carbon capture, utilization, and storage (CCUS) for achieving carbon neutrality is increasingly recognized. Carbonate minerals are currently being manufactured from the abundant calcium-containing wastes and minerals that are generated by carbon mineralization technology in industry. Among these, calcium carbonate, which is highly versatile, generally exists in three crystal forms (vaterite, aragonite, and calcite). These three crystal forms must be freely controllable to increase the value and range of use of calcium carbonate. In this study, the variables of concentration, temperature, pH, stirring speed, and stirring time were changed during the reaction of calcium raw material (i.e., CaCl₂) and carbon raw material (i.e., K₂CO₃). In addition, the phase composition ratios were determined by Rietveld refinement analysis using X-ray diffraction (XRD) patterns. Drawing on an extensive set of experimental data, we constructed data-driven predictive models by training and evaluating multilayer perceptron (MLP), support vector machine (SVM), random forest (RF), and decision tree (DT) algorithms. The best-performing model, selected by k-fold cross-validation, was then applied to determine the optimal operating conditions to control crystallinity. This study provides comprehensive knowledge about a system that allows industries to select, manufacture, and produce calcium carbonate in the crystal form they need. It is anticipated that using carbon mineralization technology, which is part of CCUS technology, will contribute to carbon neutrality, while alleviating waste environmental treatment costs.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100494"},"PeriodicalIF":0.0,"publicationDate":"2025-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144913318","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}

{"title":"Harnessing humidity for direct air capture: Moisture-swing sorbent design and mechanisms","authors":"Baljeet Singh,&nbsp;Zahra Eshaghi Gorji,&nbsp;Luc Charbonneau,&nbsp;Timo Repo","doi":"10.1016/j.ccst.2025.100497","DOIUrl":"10.1016/j.ccst.2025.100497","url":null,"abstract":"<div><div>Direct Air Capture (DAC) and Post-Combustion CO₂ capture (PCC) using liquid and solid amine sorbents, received enormous attention due to worsening weather and climate change. Enhancing the efficiency of CO₂ capture and removal technologies is crucial, with a primary focus on reducing the energy demand for continuous capture-release cycles. Low-energy CO₂ removal strategies offer promising durability and low operational costs, and a low levelized cost per ton of CO₂ removal is preferred for large-scale implementation. This review highlights low-energy CO₂ removal approaches, such as moisture/humidity swing sorbents. This discussion covers the influence of structural and molecular characteristics, the effect of counter anions on CO₂ removal efficiency and kinetics, the impact of different operational factors on performance, and the long-term stability of these materials. Continuous exploration and optimization of these materials and methods are vital for advancing the moisture swing method, contributing to global efforts to combat climate change and promoting environmental sustainability. Finally, recommendations are provided for the design of innovative materials.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100497"},"PeriodicalIF":0.0,"publicationDate":"2025-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145096441","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}

{"title":"Kinetic model describing the effect of amine loading and temperature on CO2 capture by solid amine adsorbent","authors":"Shun Wang,&nbsp;Mengyin Xie,&nbsp;Shujuan Wang,&nbsp;Yuqun Zhuo","doi":"10.1016/j.ccst.2025.100491","DOIUrl":"10.1016/j.ccst.2025.100491","url":null,"abstract":"<div><div>The increasing CO₂ concentration in atmosphere leads to significant ecological changes, and the control of CO₂ emissions has been a major concern worldwide. Amine-functionalized adsorbents are promising because they have high CO₂ adsorption capacity, moderate adsorption heat and strong water resistance. Adsorption kinetics is a key performance parameter and facilitates the cognizance of microscopic CO₂ adsorption process. A novel kinetic model was proposed, which categorized the amines of solid amine adsorbents into two regions: the open amine region and the closed amine region. Different from the open amine region, CO₂ adsorption by amines in the closed amine region was significantly influenced by diffusion. The model could elucidate the effect of amine loading and temperature on CO₂ adsorption. When amine loading was below the theoretical maximum loading, the CO₂ adsorption capacity and the N efficiency gradually increased with the rise of amine loading. Nevertheless, as the amine loading further increased, the adsorption capacity decreased instead. CO₂ adsorption by solid amines was not affected by external diffusion, but was significantly affected by internal diffusion. The percentage of closed amine region of adsorbents with high amine loading was large, CO₂ needed to diffuse slowly into this region, leading to a small CO₂ adsorption capacity at low temperature. When the amine loading was less than 0.5, the CO₂ adsorption rate stayed almost the same. The model is instructive for the targeted preparation of solid amine adsorbents with fast adsorption rates.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100491"},"PeriodicalIF":0.0,"publicationDate":"2025-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144913466","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}

{"title":"Experimental investigation and techno-economic assessment of oilfield brine-derived carbonates for calcium looping CO2 capture","authors":"Rufan Zhou ,&nbsp;Chunqing Jiang ,&nbsp;Rafal Gieleciak ,&nbsp;Lava Kumar Pillari ,&nbsp;Lukas Bichler","doi":"10.1016/j.ccst.2025.100489","DOIUrl":"10.1016/j.ccst.2025.100489","url":null,"abstract":"<div><div>Flowback and produced water (FPW) from hydraulic fracturing operations of tight hydrocarbon reservoirs has attracted significant research interest, particularly regarding its treatment and the recovery of valuable minerals. In this study, a simple and sustainable method was developed to precipitate calcium (Ca), magnesium (Mg), and strontium (Sr) carbonates from a high salinity FPW using NH₃ or NaOH and CO₂-containing flue gas. The precipitated solids and the treated FPW solution were subjected to various characterization techniques to evaluate the properties of the solids and the efficiency of the precipitation method. The precipitated carbonate minerals were further investigated as sorbents for CO₂ capture in the calcium looping process, demonstrating a substantial carbon capture capacity of approximately 0.3 kg CO₂/kg solid sample. Moreover, a series of detailed process simulations and economic analysis were performed to further evaluate the potential of using solid precipitates from FPW in the calcium looping process. Two different operating modes and multiple cases of calcium looping using solid sorbents from FPW, integrated with renewable energy, were thoroughly studied. The economic analysis of this integrated technology showed a relatively comparable levelized cost of carbon capture, at less than $200 per tonne of CO₂ captured. The techno-economic analysis of the overall process demonstrated the potential of the calcium looping process with carbonate precipitates from produced water as a possible approach for decarbonization and energy transition in the oil and gas industry.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100489"},"PeriodicalIF":0.0,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144889727","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}

{"title":"Experimental and numerical investigation of the morphological changes of a natural limestone-based CO2 sorbent over repeated carbonation-calcination cycles","authors":"Maximilian Krödel,&nbsp;Dominic Spescha,&nbsp;Agnieszka Kierzkowska,&nbsp;Felix Donat,&nbsp;Christoph R. Müller","doi":"10.1016/j.ccst.2025.100486","DOIUrl":"10.1016/j.ccst.2025.100486","url":null,"abstract":"<div><div>Morphological changes of natural limestone-based CO₂ sorbents during the cyclic transition between CaO and CaCO₃ affect their carbonation rate and cyclic CO₂ uptake. We examine the evolution of the pore structure of Havelock limestone during carbonation in the ranges (I) 2–100 nm, (II) 200–3000 nm and (III) &gt; 3000 nm with unprecedented detail, and correlate morphological changes with the observed carbonation rate. Pores of region (I) are fully filled with CaCO₃ at a CaO conversion &gt; 60 % (1st cycle), leading to a loss of ∼ 90 % of the total surface area of the sorbent, whereas pores of region (II) are only partially filled, and pores of region (III) remain largely unaffected. Throughout the carbonation reaction in the 1st and 10th cycle, the observed carbonation rate decreases linearly with the decreasing total surface area of the sorbent. Supported by kinetic and morphological modelling, our findings challenge the widely used concept of a CaCO₃ product layer of critical thickness limiting CO₂ diffusion to CaO, implying that the reaction is limited by diffusion as soon as the surface of CaO is fully covered with CaCO₃ crystallites. Our results further provide a perspective on the design of efficient CaO-based sorbents by tuning their pore diameter to be larger than &gt; 100 nm, such that the pore volume (and the respective surface area) can be largely regenerated over cycling, in turn yielding a high cyclic CO₂ uptake.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"16 ","pages":"Article 100486"},"PeriodicalIF":0.0,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144879249","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}