Carbon Capture Science & Technology最新文献

{"title":"Molecular insights into the role of kerogen in retention of geologically sequestered CO₂ in shale formations during leakage scenarios","authors":"Zikir A. Kemala ,&nbsp;Manav Kakkanat ,&nbsp;Andrey G. Kalinichev ,&nbsp;Narasimhan Loganathan ,&nbsp;Juliana Zaini ,&nbsp;Malik M. Nauman ,&nbsp;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}

{"title":"Engineered nanoporous sorbents for gaseous fluorocarbons related adsorption applications","authors":"Jian Shen ,&nbsp;Chaoxing Li ,&nbsp;Yongqi Liu ,&nbsp;Mingliang Yang ,&nbsp;Qiongzhi Zhou ,&nbsp;Fei Kang ,&nbsp;Xiaohong Zheng ,&nbsp;He Zhao ,&nbsp;Sandip Sabale ,&nbsp;Deok-kee Kim ,&nbsp;Yiming Li ,&nbsp;Jian Xiong ,&nbsp;Qiangying Zhang ,&nbsp;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}

{"title":"Next-Generation Cu-MOF-based electrocatalysts for CO2 reduction: Bridging mechanistic insights and rational design","authors":"Hafiz Muhammad Waqar Abid ,&nbsp;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 (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.</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}

{"title":"Innovative high temperature heat pump concepts for an economic decarbonization of a carbon capture unit","authors":"Shashank Singh Rawat,&nbsp;Frederico Gomes Fonseca,&nbsp;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}

{"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 ,&nbsp;Lei Liu ,&nbsp;Hanzi Liu ,&nbsp;Xuancan Zhu ,&nbsp;Zhiqiang Sun","doi":"10.1016/j.ccst.2025.100520","DOIUrl":"10.1016/j.ccst.2025.100520","url":null,"abstract":"<div><div>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 <em>g</em>⁻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.</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}

{"title":"Advances in concurrent CO2 sequestration and heavy metal mobilization during fly ash carbonation: A review","authors":"Qingqin Wang,&nbsp;Zichen Cao,&nbsp;Qingqing Li,&nbsp;Bing Song","doi":"10.1016/j.ccst.2025.100519","DOIUrl":"10.1016/j.ccst.2025.100519","url":null,"abstract":"<div><div>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.</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}

{"title":"Feasibility assessment of a spray tower for gas-liquid reactive precipitation in CO2 capture","authors":"Robert Kiefel ,&nbsp;Jonas Görtz ,&nbsp;Jan Haß ,&nbsp;Julius Walorski ,&nbsp;Falk Zimmer ,&nbsp;Andreas Jupke","doi":"10.1016/j.ccst.2025.100509","DOIUrl":"10.1016/j.ccst.2025.100509","url":null,"abstract":"&lt;div&gt;&lt;div&gt;The industrial deployment of &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;/mrow&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; capture technologies for purifying gases with low &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;/mrow&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; 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 &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;/mrow&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; 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 &lt;span&gt;&lt;math&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;HCO&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;mo&gt;−&lt;/mo&gt;&lt;/msubsup&gt;&lt;/math&gt;&lt;/span&gt; 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 &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;/mrow&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; 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 &lt;span&gt;&lt;math&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;/mrow&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;−&lt;/mo&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;&lt;/span&gt;-precipitating system (&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Ba&lt;/mi&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mtext&gt;OH&lt;/mtext&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;) and a non-precipitating system (&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;NaOH&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;), 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 &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mi&gt;GBIG&lt;/mi&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; system demonstrates superior &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;/mrow&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; capture efficiency relative to the &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mi&gt;Ba&lt;/mi&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mtext&gt;OH&lt;/mtext&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; 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}

{"title":"Techno-economic analysis of packed bed and structured adsorbent for direct air capture","authors":"Paul de Joannis ,&nbsp;Christophe Castel ,&nbsp;Mohamed Kanniche ,&nbsp;Eric Favre ,&nbsp;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 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.</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}

{"title":"Natural carbonation in alkali basalts: Geochemical evolution of Ca–Mg–Fe carbonates at Sverrefjellet, Svalbard","authors":"Andrea Pierozzi ,&nbsp;Niamh Faulkner ,&nbsp;Adrienn Maria Szucs ,&nbsp;Luca Terribili ,&nbsp;Melanie Maddin ,&nbsp;Federica Meloni ,&nbsp;Kavya Devkota ,&nbsp;Kristina Petra Zubovic ,&nbsp;Paul C. Guyett ,&nbsp;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_0.05Mg_0.95CO₃) to Ca-enriched rims (Ca_0.40Mg_0.60CO₃), reflecting evolving fluid chemistry. Fe-rich nodules (Ca_0.10Mg_0.50Fe_0.40CO₃) 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 (Ca_0.65–0.58Mg_0.35–0.42CO₃), transitioning outward to magnesite (Ca_0.10Mg_0.90CO₃) and ferroan magnesite (Ca_0.10Mg_0.50Fe_0.40CO₃). 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.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100510"},"PeriodicalIF":0.0,"publicationDate":"2025-09-04","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}

{"title":"Accelerating CO2 sequestration in cementitious materials using carbonic anhydrase: Experimental insights into performance and mechanisms","authors":"Xiulin Chen,&nbsp;Zhidong Zhang,&nbsp;Ueli Angst","doi":"10.1016/j.ccst.2025.100511","DOIUrl":"10.1016/j.ccst.2025.100511","url":null,"abstract":"<div><div>Increasing atmospheric CO₂ levels require innovative mitigation strategies. Cementitious materials offer significant potential for CO₂ sequestration through carbonation. This study investigates the application of carbonic anhydrase (CA), an enzyme that catalyzes CO₂ hydration, to accelerate CO₂ sequestration in cementitious materials. We applied pH monitoring and p-NPA assay to evaluate CA activity under artificial cementitious environments. The results showed that CA activity significantly decreased at pH 13 but remained stable at pH below 12, suggesting potential applications of CA in lower-pH systems, such as demolished concrete, mineral waste, or cementitious materials with a low clinker content. Mixing CA directly into fresh cement pastes showed more carbonates formed and a higher reduction in pore volume than the control groups, demonstrating that CA accelerated early-stage CO₂ sequestration. When spraying the CA solution on crushed cement paste, we observed a dense layer of calcite on the surfaces of cement paste particles, meaning that early-stage carbonation resulted in a higher carbonate content than the control samples, particularly for smaller particles with larger surface areas. However, the carbonation efficiency decreased at the later stage, which is likely due to CA deactivation or surface densification limiting ions diffusion, reducing further carbonation enhancement at later stages. This study highlights the potential of CA to accelerate CO₂ sequestration in cementitious materials while emphasizing the challenges of high pH and complex ionic composition for CA performance. The findings suggest the need for stabilizing the enzyme’s activity or applying CA to low-clinker cementitious materials, and partially carbonated materials, such as recycled concrete aggregates, for CO₂ sequestration.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"17 ","pages":"Article 100511"},"PeriodicalIF":0.0,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145027389","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}