{"title":"Analysis of new strategies integrating bipolar membrane electrodialysis and absorption systems in DAC applications","authors":"Grazia Leonzio , Lei Xing , Nilay Shah","doi":"10.1016/j.ccst.2026.100579","DOIUrl":"10.1016/j.ccst.2026.100579","url":null,"abstract":"<div><div>Solvent-based carbon dioxide capture technologies remain among the most promising capture strategies but conventional thermal regeneration methods are hindered by significant drawbacks. In this context, electrochemical regeneration, particularly through the bipolar membrane electrodialysis, offers potential advantages. However, its application is challenged by carbon dioxide bubble formation in the acid compartment, which increases energy requirements. To address this issue, a novel process is proposed in which carbonates in the rich solvent react with weak organic acids to release carbon dioxide while forming acid salts treated in the electrodialysis unit, enabling simultaneous the regeneration of both acid and solvent. To date, comprehensive economic and environmental assessments of such approaches are lacking in the state-of-the-art. This study aims to fill that gap by simulating both the conventional process and alternative pathways based on formic acid and a formic/acetic acid mixtures. Comprehensive material and energy balances are established, alongside detailed evaluations of capital and operating expenditures, and the environmental impact are conducted through life cycle assessment implemented in OpenLCA. Although the alternative processes exhibit higher energy consumption (2314 kWh/tonCO₂ vs 1907 kWh/tonCO₂ with formic acid, and 1943 kWh/tonCO₂ with the acid mixture), the conventional route remains more favorable in terms of both overall cost and environmental impact. Specifically, the total cost and climate change impact of the conventional capture process are estimated to be 480 $/tonCO₂ and –0.9593 kgCO₂<sub>eq</sub>/kgCO₂, respectively. On the other hand, the alternative process using formic acid and the mixture acid incur higher costs of 510 $/tonCO<sub>2</sub> and 519 $/tonCO<sub>2</sub> with corresponding environmental impacts of -0.9378 kgCO<sub>2eq</sub>/kgCO<sub>2</sub> and 0.9238 kgCO<sub>2eq</sub>/kgCO<sub>2</sub>, respectively. Further optimization of the conventional process, particularly in mitigating carbon dioxide bubble formation, appears essential to fully exploit its economic and environmental potential.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100579"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146169951","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}
Yan Tian , Chao Li , Da Li , Hongxu Lu , Xiaoyu Li , Yujie Feng
{"title":"Enhanced CO2 electromethanogenesis using biogas over pure CO2 as MES feedstock: Performance and microbial mechanisms","authors":"Yan Tian , Chao Li , Da Li , Hongxu Lu , Xiaoyu Li , Yujie Feng","doi":"10.1016/j.ccst.2026.100577","DOIUrl":"10.1016/j.ccst.2026.100577","url":null,"abstract":"<div><div>Microbial electrosynthesis (MES) has shown excellent CO<sub>2</sub>-to-CH<sub>4</sub> activity with pure CO<sub>2</sub> stream. However, its performance and electron transfer pathway has not been deeply unveiled when biogas was used as MES feedstock. In this work, mimic biogas composed of 60% CH<sub>4</sub> and 40% CO<sub>2</sub> was fed into biocathode MES (–1.0 V vs. Ag/AgCl) to evaluate its efficiency of biogas upgrading. Compared to pure CO<sub>2</sub>-fed MES, the faradaic efficiency of biogas-fed MES was increased by 15.1% with 1.34-fold of conversion rate. Metagenomic sequencing and qPCR analysis revealed that the lower CO<sub>2</sub> content under biogas condition stimulated the enrichment of electroactive- methanogens and bacteria, which primarily facilitated electron transfer during CO<sub>2</sub> conversion. Notably, it was proposed that the spatial consortium of “methanogens–electroactive bacteria,” rather than the methanogen abundance within the biofilm, contributed to the CO<sub>2</sub>-to-CH<sub>4</sub> performance. Overall, these results indicate that low CO<sub>2</sub> partial pressure in biogas enhances the activity of the methanogenic biocathode for biogas upgrading, rather than inhibiting methanogenesis. This study provides comprehensive insights into the mechanism of electromethanogenesis using biogas as MES feedstock. Future efforts should focus on the development of large-scale, practical continuous-flow systems to advance this technology.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100577"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170004","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":"Direct air capture (DAC) and CO2 sequestration with waste brine using a novel sorbent at ambient temperature","authors":"Xinkai Wu , Hao Chen , Haibo Liu, Arup K. SenGupta","doi":"10.1016/j.ccst.2026.100584","DOIUrl":"10.1016/j.ccst.2026.100584","url":null,"abstract":"<div><div>There is a global consensus that CO<sub>2</sub> capture and sequestration should continue at an accelerated pace to meet the IPCC (Intergovernmental Panel on Climate Change) recommendation in lowering the CO<sub>2</sub> concentration in the atmosphere. In recent years, deployment of direct air capture (DAC) has been on the rise through use of solid sorbents. In this study, we present for the first time a new DAC process that eliminates the need for geological storage and thermal desorption. A hybrid polymeric ion exchanger for decarbonization (DeCarbon-HIX), that is robust and durable, forms the heart of the process. Besides high CO<sub>2</sub> capture capacity from the atmosphere, the DeCarbon-HIX sorbent is amenable to regeneration with waste brine solution (e.g., produced water) containing Ca<sup>2+</sup> whereby CO<sub>2</sub> is mineralized as solid, innocuous CaCO<sub>3</sub>(s). Note that other recently developed DAC processes, namely, moisture swing DAC and electrochemistry-driven processes, operate without thermal energy but require CO<sub>2</sub> storage. This new avenue for DAC offers great opportunities to capture CO<sub>2</sub> in countries and islands where reliable geological storage is non-existent. This carbon dioxide removal methodology can be rapidly scaled up in many regions that are currently inaccessible to DAC.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100584"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147385304","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":"A computational study of electric field-controlled CO2 Capture using earth-abundant metals","authors":"Lakshmi Anil, Kulbir Kaur Ghuman","doi":"10.1016/j.ccst.2026.100585","DOIUrl":"10.1016/j.ccst.2026.100585","url":null,"abstract":"<div><div>With the growing urgency to combat climate change, developing energy-efficient and tunable direct air capture (DAC) technologies for CO<sub>2</sub> removal has become an urgent scientific and engineering challenge. This study explores a novel strategy that leverages external electric fields (EFs) and surface charges to modulate CO<sub>2</sub> adsorption and desorption on low-cost, earth-abundant metal surfaces with varying d-orbital occupancies. Using Density Functional Theory (DFT), we systematically investigated Cu (111), Fe (110), and Zn (0001) surfaces, representing moderate, high, and inert reactivity, respectively.</div><div>Without external stimuli, Fe (110) intrinsically chemisorbs CO<sub>2</sub>, while Cu (111) and Zn (0001) surfaces exhibit only weak physisorption. Upon application of an EF and excess surface charge, all three surfaces show enhanced CO<sub>2</sub> activation, with the effect being most pronounced on Cu (111) surface. The application of an EF leads to a transition from physisorption to chemisorption, accompanied by significant molecular activation. Reversing the field with a modest potential (∼ -2 V) enables efficient CO<sub>2</sub> desorption, completing a low-energy capture-release cycle. In contrast, Fe binds CO<sub>2</sub> too strongly, rendering desorption ineffective even under a strong reverse field (-40 V), while Zn remains largely unresponsive due to filled d-orbitals, showing minimal activation for CO<sub>2</sub> adsorption even at high field strengths (30 V).</div><div>Among the three, Cu (111) emerges as the most promising candidate for electrically tunable CO<sub>2</sub> capture, offering a balance between reactivity and reversibility due to its nearly filled d-band configuration. By elucidating the crucial roles of d-orbital occupancy and electric field sensitivity, this work presents electrically modulated adsorption and desorption as an effective carbon capture mechanism that eliminates the need for chemical functionalization, surface modification, or energy-intensive thermal or pressure processes. This approach opens new pathways for designing tunable CO<sub>2</sub> capture systems through targeted material selection and electric field engineering.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100585"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146169950","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":"Investigating carbon sequestration in cementitious mortars with low-carbon binders and carbonated water","authors":"Aswathy Rajendran, Sripriya Rengaraju, Abir Al-Tabbaa","doi":"10.1016/j.ccst.2026.100570","DOIUrl":"10.1016/j.ccst.2026.100570","url":null,"abstract":"<div><div>The use of carbonated water in cementitious systems as a carbon sequestration strategy is promising, offering operational simplicity and high CO<sub>2</sub> binding efficiency compared to approaches such as gaseous CO<sub>2</sub> injection and carbonation curing. However, its application in low-carbon cement systems, particularly emerging binders such as limestone calcined clay cement (LC<sup>3</sup>), remains underexplored. As the shift to low-carbon binders is critical for reducing embodied carbon in cement, it is essential to understand their interactions with carbonated water, given their distinct reactivity, pH evolution, and fresh-state behaviour. This study systematically investigates the effects of carbonated water on conventional low-carbon binders (Slag-50% and Slag-80%), emerging LC<sup>3</sup>, and OPC mortars. Evaluations covered fresh-state properties, mechanical performance, durability (sorptivity and porosity), and microstructural evolution at early and later ages. Results show the strongest interaction of carbonate ions with C<sub>3</sub>A and its hydration products, with CO<sub>2</sub> binding governed by the nature of early hydrates and pH conditions. Contrary to the hypothesis that high-calcium systems such as OPC are most favourable for CO<sub>2</sub> binding, they exhibited reduced strength and durability. In contrast, LC<sup>3</sup> and Slag-50% demonstrated the greatest benefits, with improved CO<sub>2</sub> binding, shortened setting times, enhanced strength and reduced sorptivity and porosity. Microstructural analysis confirmed CO<sub>2</sub> binding predominantly influenced calcium-silicate-hydrate gels with minimal calcite formation. Overall, carbonated water emerges as a practical pathway to improve performance while enabling additional CO<sub>2</sub> binding in LC<sup>3</sup> and slag-50% cement systems, reinforcing their superior potential for carbon sequestration to OPC.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100570"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145972756","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":"Modifying CO2 absorption-desorption: A comprehensive review of advances in process design, solvent engineering, energy integration, and operational optimisation","authors":"Meisam Ansarpour, Tohid N. Borhani","doi":"10.1016/j.ccst.2025.100548","DOIUrl":"10.1016/j.ccst.2025.100548","url":null,"abstract":"<div><div>Efficient carbon capture through CO<sub>2</sub> absorption-desorption processes is crucial for mitigating climate change and meeting global greenhouse gas reduction targets. This comprehensive review synthesises over a decade of advancements addressing the technical and economic challenges pertinent to absorption-based carbon capture. It focuses on four critical aspects: process configuration, solvent innovation, energy integration, and operational optimisation. The review evaluates emerging process designs that improve CO<sub>2</sub> capture efficiency and reduce energy penalties, including absorber intercooling, advanced stripper configurations, and solvent recycle strategies. Further, it critically assesses novel solvents and solvent mixtures such as amines, ionic liquids, deep eutectic solvents, biphasic systems, and nanofluids, aimed at enhancing solvent stability, absorption capacity, and cyclic performance. The paper highlights energy-saving techniques through heat and mass integration as well as emerging heat pump technologies that minimise heat loss, thereby improving overall system sustainability. Additionally, this review covers the expanding use of computational methods, including experimental design, machine learning, artificial intelligence, and metaheuristic optimisation, to identify optimal operating conditions and improve process scalability. Unlike previous reviews, this study integrates advances across multiple disciplines include process engineering, solvent chemistry, energy management, and computational optimisation by providing a holistic view of current progress and remaining gaps. It offers practical insights and recommendations to guide future research and accelerate the industrial deployment of cost-effective and energy-efficient CO<sub>2</sub> capture technologies. The novelty and urgency of this synthesis lie in its multidisciplinary approach combining experimental, theoretical, and computational studies to address persistent challenges and future opportunities in carbon capture science.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100548"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145787735","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}
Bo Wang , Yuanhao Chang , Rui Ma , Xiangzeng Wang , Fujie Jiang , Fanhua Zeng
{"title":"Deciphering salt precipitation in saline aquifer carbon sequestration: Insight from microfluidic and molecular perspectives","authors":"Bo Wang , Yuanhao Chang , Rui Ma , Xiangzeng Wang , Fujie Jiang , Fanhua Zeng","doi":"10.1016/j.ccst.2026.100574","DOIUrl":"10.1016/j.ccst.2026.100574","url":null,"abstract":"<div><div>Saline aquifer carbon sequestration is a key strategy for mitigating greenhouse gas emissions and supporting energy sustainability. However, salt precipitation induced by CO<sub>2</sub> injection can substantially impair storage efficiency. A clear understanding of salt precipitation dynamics is therefore essential for predicting crystal distribution and assessing pore-scale structural damage. In this study, microfluidic technology combined with image-based quantitative pore-scale analysis was used to systematically investigate salt precipitation behavior. Molecular dynamics (MD) simulations were performed to complement microfluidic experiments and to elucidate the molecular mechanisms underlying ion interaction and salt crystallization. The results indicate that salt precipitation proceeds through five stages: nucleation, migration, growth, retention, and blockage. Nucleation occurs in two distinct structural forms at four characteristic locations, including bulk crystals in high-saturation regions and porous aggregated crystals in low-saturation areas. Crystal migration is governed by the availability of brine as a transport medium and by weak crystal–surface adhesion. Retention and blockage develop through both in-situ and ex-situ modes, with hygroscopicity, concentration gradients, and capillary backflow playing critical roles in ex-situ precipitation. MD simulations revealed salt precipitation features consistent with those observed in the microfluidic experiments and confirmed that nucleation preferentially occurs at gas-liquid interfaces and three-phase contact regions, driven by ion aggregation and surface interactions. In porous media, both brine evaporation and salt crystallization follow a three-stage process, which significantly impacts pore structure and permeability. This study provides new mechanistic insights into salt-induced pore blockage and offers guidance for optimizing CO<sub>2</sub> injection strategies, thereby advancing the understanding of salt precipitation processes in subsurface gas storage and related engineering applications.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100574"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146073652","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}
Hyunji Lim , Kwanghwi Kim , Hyun Sic Park , Jo Hong Kang , Jinwon Park , Hojun Song
{"title":"Continuous CO2 capture using a hollow fiber membrane contactor with stripper regeneration: Bench-scale validation with amino acid salt–piperazine absorbents","authors":"Hyunji Lim , Kwanghwi Kim , Hyun Sic Park , Jo Hong Kang , Jinwon Park , Hojun Song","doi":"10.1016/j.ccst.2026.100573","DOIUrl":"10.1016/j.ccst.2026.100573","url":null,"abstract":"<div><div>Membrane contactor technologies offer a promising solution for CO<sub>2</sub> capture; however, their optimization remains challenging. This study explored the CO<sub>2</sub> absorption and desorption performances in a hybrid process involving a hollow fiber membrane contactor (HFMC) and a stripping tower in a bench-scale system. Three absorbents [2.5 M monoethanolamine (MEA), potassium serinate + piperazine (PSZ), and potassium alaninate + piperazine (PAZ)] were tested at total absorbent molarity under varying liquid flow rates to evaluate their CO<sub>2</sub> removal efficiencies, absorption fluxes, and overall mass transfer coefficients. The results showed that PAZ exhibited the highest CO<sub>2</sub> capture performance, while also significantly reducing the regeneration energy and membrane wetting. The PAZ absorbent maintained a stable performance during simultaneous operation, with a 73 % reduction in crossover volume and a 31 % decrease in the regeneration energy compared to MEA. The membrane contactor process demonstrated enhanced characteristics compared to a conventional packed column under similar gas flow rates, with a four times higher CO<sub>2</sub> absorption rate and a 79 % smaller unit volume. Furthermore, long-term oxidative degradation tests confirmed the durability of the PAZ absorbent. Overall, this study demonstrates the potential of combining HFMCs with optimized PAZ absorbents to enhance the CO<sub>2</sub> capture efficiency and minimize operational challenges, leading to a more compact and efficient carbon capture process.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100573"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146073655","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}
Binhai Cheng , Zhenyu Jin , Xin Meng , Wei Wang , Yi Lv , Ming Zhao
{"title":"Catalytic cycloaddition of CO2 and epoxides by sustainable metal-free N,O-enriched hydrochar","authors":"Binhai Cheng , Zhenyu Jin , Xin Meng , Wei Wang , Yi Lv , Ming Zhao","doi":"10.1016/j.ccst.2026.100578","DOIUrl":"10.1016/j.ccst.2026.100578","url":null,"abstract":"<div><div>The cycloaddition of CO₂ and epoxides to produce cyclic carbonates offers an atom-economical route for carbon utilization, yet its industrial implementation is hindered by the scarcity of sustainable, efficient, and cost-effective catalysts. We herein develop a metal-free N/O-enriched hydrochar (NO-HC) through a one-pot synthesis using nitrogen-rich biomass precursors. The optimized NO-HC<sub>100</sub> catalyst achieves 95 % cyclic carbonate yield under solvent- and co-catalyst-free conditions, exhibiting exceptional substrate generality. It demonstrated that the improved catalytic performance is attributed to the abundant acid and base active sites that are dominated by the doping oxygen and nitrogen groups, respectively. This conclusion can be extended to the widely existing actual biomass, considering the composition and nitrogen content of biomass, as well as the corresponding pre-treatment methods (e.g., deash). This work provides a circular economy paradigm that synergistically valorizes nitrogen-containing biomass into functional carbocatalysts while converting CO₂ into value-added chemicals, achieving dual carbon mitigation through waste-to-resource conversion and greenhouse gas utilization.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100578"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146169944","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}
Bennet Nii Tackie-Otoo , Mobeen Murtaza , Mahmoud Abdelnaby , Sagheer A. Onaiz , Shirish Patil , Muhammad Shahzad Kamal , Mohamed Mahmoud , Arshad Raza , Amro Elsayed
{"title":"Zeolitic imidazolate framework/graphene hybrid nanocomposites for downhole CO2/H2 separation during in-situ hydrogen production from hydrocarbon reservoirs","authors":"Bennet Nii Tackie-Otoo , Mobeen Murtaza , Mahmoud Abdelnaby , Sagheer A. Onaiz , Shirish Patil , Muhammad Shahzad Kamal , Mohamed Mahmoud , Arshad Raza , Amro Elsayed","doi":"10.1016/j.ccst.2025.100565","DOIUrl":"10.1016/j.ccst.2025.100565","url":null,"abstract":"<div><div>Selective CO<sub>2</sub> separation from H₂-rich streams is crucial for advancing in-situ hydrogen production from depleted natural gas reservoirs. This study investigates pristine-graphene-based nanocomposites of ZIF-8 and ZIF-67 as solid sorbents for high-pressure CO<sub>2</sub>/H<sub>2</sub> separation. Graphene@ZIF-8 and Graphene@ZIF-67 were synthesized via a modified sonochemical route that enabled uniform ZIF crystal growth on graphene. XRD confirmed complete retention of the sodalite topology with no impurity phases. SEM and BET analyses showed that incorporating graphene increased the BET surface area of ZIF-8 from 1284 to 1471 m<sup>2</sup>/g (+15%) and ZIF-67 from 1116 to 1413 m<sup>2</sup>/g (+27%), while also increasing total pore volume by ∼10-16%. CO<sub>2</sub> adsorption improved substantially, with Graphene@ZIF-8 (75 cm<sup>3</sup>/g) and Graphene@ZIF-67 (65 cm<sup>3</sup>/g) exhibiting ∼2× higher uptake than their pristine ZIF counterparts (38 and 25 cm<sup>3</sup>/g, respectively). Langmuir monolayer capacities similarly increased from 105 to 404 cm<sup>3</sup> (+285%) for ZIF-8 and from 48 to 354 cm<sup>3</sup> (+637%) for ZIF-67 upon graphene hybridization. In contrast, H<sub>2</sub> uptake remained lower than CO<sub>2</sub>, producing enhanced CO<sub>2</sub>/H<sub>2</sub> selectivity; Graphene@ZIF-8 achieved a maximum selectivity of ∼11, compared to ∼10 for ZIF-8 and <4 for ZIF-67. These improvements demonstrate that pristine-graphene-supported ZIF nanocomposites provide significantly enhanced adsorption capacity and selectivity, making them strong candidates for CO<sub>2</sub> capture from H<sub>2</sub>-rich gas streams in subsurface hydrogen production.</div></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"18 ","pages":"Article 100565"},"PeriodicalIF":0.0,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145880952","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}