Pub Date : 2026-03-01Epub Date: 2026-02-02DOI: 10.1016/j.jcou.2026.103348
Mohammad Azadi Tabar , Esther Pancione , Sunil Adavanal Peter , Joeri F.M. Denayer
In this work, a four-column Vacuum Pressure Swing Adsorption (VPSA) pilot unit was constructed and tested for biogas upgrading. The columns were packed with the carbon molecular sieve Shirasagi CT-350 (CMS) adsorbent. A 12-steps process configuration was designed to upgrade a synthetic mixture of CH4/CO2 (60/40 %vol), representing biogas, to biomethane. Experiments and simulations were carried out at room temperature (298 K) with an adsorption pressure of 4 bar, using a non-isothermal dynamic Aspen Adsorption™ model to support process interpretation. The configuration performance was evaluated for two feed flowrates of 2 SL/min and 3 SL/min, two vacuum pressures of 0.1 bar and 0.2 bar, while variating the evacuation time from 55 s to 700 s. Results indicated that at lower feed flowrates, higher CH4 purity and recovery were achieved at the cost of higher energy consumption. Additionally, longer vacuum times (corresponding to longer adsorption times) reduced the total energy consumption. The best case of the experimental campaign, at vacuum pressure of 0.2 bar and feed flowrate of 3 SL/min, achieved a raffinate stream with 95.9 % CH4 purity and 97.9 % CH4 recovery, while simultaneously producing an extract stream with 96.7 % CO2 purity and 93.6 % CO2 recovery. These results demonstrate the high efficiency and potential of CMS-based multi-column VPSA configurations for upgrading biogas to biomethane while generating a high-purity CO2 co-product.
{"title":"Four-column Vacuum Pressure Swing Adsorption for biogas upgrading with co-production of high-purity biogenic CO2: Experimental and simulation study","authors":"Mohammad Azadi Tabar , Esther Pancione , Sunil Adavanal Peter , Joeri F.M. Denayer","doi":"10.1016/j.jcou.2026.103348","DOIUrl":"10.1016/j.jcou.2026.103348","url":null,"abstract":"<div><div>In this work, a four-column Vacuum Pressure Swing Adsorption (VPSA) pilot unit was constructed and tested for biogas upgrading. The columns were packed with the carbon molecular sieve Shirasagi CT-350 (CMS) adsorbent. A 12-steps process configuration was designed to upgrade a synthetic mixture of CH<sub>4</sub>/CO<sub>2</sub> (60/40 %vol), representing biogas, to biomethane. Experiments and simulations were carried out at room temperature (298 K) with an adsorption pressure of 4 bar, using a non-isothermal dynamic Aspen Adsorption™ model to support process interpretation. The configuration performance was evaluated for two feed flowrates of 2 SL/min and 3 SL/min, two vacuum pressures of 0.1 bar and 0.2 bar, while variating the evacuation time from 55 s to 700 s. Results indicated that at lower feed flowrates, higher CH<sub>4</sub> purity and recovery were achieved at the cost of higher energy consumption. Additionally, longer vacuum times (corresponding to longer adsorption times) reduced the total energy consumption. The best case of the experimental campaign, at vacuum pressure of 0.2 bar and feed flowrate of 3 SL/min, achieved a raffinate stream with 95.9 % CH<sub>4</sub> purity and 97.9 % CH<sub>4</sub> recovery, while simultaneously producing an extract stream with 96.7 % CO<sub>2</sub> purity and 93.6 % CO<sub>2</sub> recovery. These results demonstrate the high efficiency and potential of CMS-based multi-column VPSA configurations for upgrading biogas to biomethane while generating a high-purity CO<sub>2</sub> co-product.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103348"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-02-14DOI: 10.1016/j.jcou.2026.103360
Xinxin Fan , Zhian Fang , Yanting Ouyang , Lu Qian , Xiyue Li , Xiaoyu Chen , Biying Xie , Chunyi Wang , Tiejun Lu , Long Xi , Zhenwen Qiu , Alan Xiaodong Zhuang , Qingguo Li
Improving drug loading and dissolution of poorly water-soluble active pharmaceutical ingredients (APIs) remains a major challenge in formulation development. Here, we integrate atomic force microscopy (AFM) adhesion-force profiling with supercritical antisolvent fluidized-bed (SAS-FB) technology to establish a predictive framework for drug–carrier selection. Enzalutamide (ENZ), a highly crystalline and poorly soluble biopharmaceutics classification system (BCS) Class II compound, was used as a stringent model drug. Single-particle force spectroscopy measurements quantified nanoscale interaction forces between SAS-processed ENZ microcrystals and seven carrier materials. Among these, lactose T70 exhibited the highest adhesion force, which strongly correlated with its superior encapsulation efficiency (EE = 92.7 %) under identical SAS-FB processing conditions. Statistical analysis revealed a robust linear relationship between mean adhesion force and EE (R² = 0.94453), identifying adhesion force as a quantitative predictor of drug deposition efficiency. This predictive capability was further validated using three additional model compounds (naringenin, dihydromyricetin, and luteolin). Comprehensive physicochemical characterization (SEM, PSD, EDS, DSC, XRD, FT-IR, and ¹H NMR) confirmed effective deposition of ENZ onto lactose T70, particle-size reduction, preserved chemical integrity, and SAS-induced polymorphic transformation. The optimized ENZ@SAS-FB(T70) formulation achieved a 5.5-fold increase in dissolution compared with unprocessed ENZ, attributed to uniform coating, enhanced wetting, and improved dispersion of micronized drug on the carrier surface. Collectively, this study establishes AFM-guided carrier screening as a mechanistic and efficient strategy for optimizing SAS-FB formulations. By linking nanoscale adhesion forces to macroscopic encapsulation outcomes, this framework offers a generalizable approach for accelerating the development of high-performance formulations for poorly soluble APIs.
{"title":"Integrating AFM adhesion profiling with supercritical antisolvent fluidized-bed CO₂ processing to optimise drug loading","authors":"Xinxin Fan , Zhian Fang , Yanting Ouyang , Lu Qian , Xiyue Li , Xiaoyu Chen , Biying Xie , Chunyi Wang , Tiejun Lu , Long Xi , Zhenwen Qiu , Alan Xiaodong Zhuang , Qingguo Li","doi":"10.1016/j.jcou.2026.103360","DOIUrl":"10.1016/j.jcou.2026.103360","url":null,"abstract":"<div><div>Improving drug loading and dissolution of poorly water-soluble active pharmaceutical ingredients (APIs) remains a major challenge in formulation development. Here, we integrate atomic force microscopy (AFM) adhesion-force profiling with supercritical antisolvent fluidized-bed (SAS-FB) technology to establish a predictive framework for drug–carrier selection. Enzalutamide (ENZ), a highly crystalline and poorly soluble biopharmaceutics classification system (BCS) Class II compound, was used as a stringent model drug. Single-particle force spectroscopy measurements quantified nanoscale interaction forces between SAS-processed ENZ microcrystals and seven carrier materials. Among these, lactose T70 exhibited the highest adhesion force, which strongly correlated with its superior encapsulation efficiency (EE = 92.7 %) under identical SAS-FB processing conditions. Statistical analysis revealed a robust linear relationship between mean adhesion force and EE (R² = 0.94453), identifying adhesion force as a quantitative predictor of drug deposition efficiency. This predictive capability was further validated using three additional model compounds (naringenin, dihydromyricetin, and luteolin). Comprehensive physicochemical characterization (SEM, PSD, EDS, DSC, XRD, FT-IR, and ¹H NMR) confirmed effective deposition of ENZ onto lactose T70, particle-size reduction, preserved chemical integrity, and SAS-induced polymorphic transformation. The optimized ENZ@SAS-FB(T70) formulation achieved a 5.5-fold increase in dissolution compared with unprocessed ENZ, attributed to uniform coating, enhanced wetting, and improved dispersion of micronized drug on the carrier surface. Collectively, this study establishes AFM-guided carrier screening as a mechanistic and efficient strategy for optimizing SAS-FB formulations. By linking nanoscale adhesion forces to macroscopic encapsulation outcomes, this framework offers a generalizable approach for accelerating the development of high-performance formulations for poorly soluble APIs.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103360"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170849","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-02-06DOI: 10.1016/j.jcou.2026.103342
Liangsheng He , Shengnan Yan , Zhenggui Li , Fang Chen , Qin Zhao , Hongteng Wu , Yawei Bai , Xiaolin Yang
The CaO/CaCO3 cycle system holds broad application prospects in high-temperature processes such as thermal chemical energy storage for concentrated solar power generation and CO2 capture and utilization. However, most numerical studies typically employ calcium-based particles of a single particle size, making it difficult to reflect the influence of particle size distribution on fluidization and reaction behaviour within actual systems. To elucidate the fluidization and reaction characteristics of CaO/CaCO3 in bubbling fluidized beds, this study employs polydisperse calcium-based particles as the research subject. Numerical simulations incorporating chemical reactions are conducted to investigate particle fluidization behaviour under varying gas velocities, inlet CO2 volume fractions, and dynamic operating conditions from a parameterisation perspective. By comparing different particle size combinations, characteristic parameters such as bed solid content distribution, time-averaged CO2 concentration, time-averaged axial solid content, and time-averaged velocity were analysed. Results indicate that at constant gas velocity, the bed’s CO2 adsorption efficiency gradually decreases as particle size increases from 75 μm to 136 μm. In the mixed-particle-size system, at the same gas velocity, the CaCO3 solid content in the single-particle-size bed was slightly lower than that in the mixed-particle-size bed, while the CaO solid content was higher than that in the mixed-particle-size bed. Under different inlet CO2 concentration conditions, higher CO2 concentrations led to decreases in the bed's time-averaged velocity and time-averaged axial solid content. Considering particle temperature distribution, CO2 adsorption efficiency, CaO conversion rate, and energy storage density comprehensively, the calcium-based particle system demonstrated superior overall performance when the inlet CO2 volume fraction was 0.85.
{"title":"Parametric study of CO2 capture and thermal energy storage in a CaO/CaCO3 bubbling fluidized bed with polydisperse particles","authors":"Liangsheng He , Shengnan Yan , Zhenggui Li , Fang Chen , Qin Zhao , Hongteng Wu , Yawei Bai , Xiaolin Yang","doi":"10.1016/j.jcou.2026.103342","DOIUrl":"10.1016/j.jcou.2026.103342","url":null,"abstract":"<div><div>The CaO/CaCO<sub>3</sub> cycle system holds broad application prospects in high-temperature processes such as thermal chemical energy storage for concentrated solar power generation and CO<sub>2</sub> capture and utilization. However, most numerical studies typically employ calcium-based particles of a single particle size, making it difficult to reflect the influence of particle size distribution on fluidization and reaction behaviour within actual systems. To elucidate the fluidization and reaction characteristics of CaO/CaCO<sub>3</sub> in bubbling fluidized beds, this study employs polydisperse calcium-based particles as the research subject. Numerical simulations incorporating chemical reactions are conducted to investigate particle fluidization behaviour under varying gas velocities, inlet CO<sub>2</sub> volume fractions, and dynamic operating conditions from a parameterisation perspective. By comparing different particle size combinations, characteristic parameters such as bed solid content distribution, time-averaged CO<sub>2</sub> concentration, time-averaged axial solid content, and time-averaged velocity were analysed. Results indicate that at constant gas velocity, the bed’s CO<sub>2</sub> adsorption efficiency gradually decreases as particle size increases from 75 μm to 136 μm. In the mixed-particle-size system, at the same gas velocity, the CaCO<sub>3</sub> solid content in the single-particle-size bed was slightly lower than that in the mixed-particle-size bed, while the CaO solid content was higher than that in the mixed-particle-size bed. Under different inlet CO<sub>2</sub> concentration conditions, higher CO<sub>2</sub> concentrations led to decreases in the bed's time-averaged velocity and time-averaged axial solid content. Considering particle temperature distribution, CO<sub>2</sub> adsorption efficiency, CaO conversion rate, and energy storage density comprehensively, the calcium-based particle system demonstrated superior overall performance when the inlet CO<sub>2</sub> volume fraction was 0.85.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103342"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170656","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-02-02DOI: 10.1016/j.jcou.2026.103343
P. Majidi , S. Jafarmadar , S. Fathi
The dry methane reforming process holds the potential to convert the greenhouse gas carbon dioxide into high-value-added fuels and chemicals, presenting broad application prospects in the fields of environmental protection and renewable energy. In this study, a two-stage pulsed discharge cold plasma reactor was experimentally investigated at ambient temperature and atmospheric pressure. The primary products of this process were syngas (CO and H₂), with smaller quantities of C₂Hᵧ compounds (y = 2, 4, or 6) also produced as by-products. This research aims to examine and compare a single-stage plasma system with a two-stage system. The results demonstrate that a significant improvement in methane conversion and hydrogen selectivity is achieved when the plasma energy is discharged across two stages. This performance enhancement is attributed to the presence of hydrogen generated in the second plasma stage. These findings indicate that plasma power alone is not the sole factor determining optimal performance; rather, the method of its delivery can profoundly influence the conversion of methane and carbon dioxide, product yields, and energy conversion efficiency. In this configuration, the hydrogen produced in the first stage promotes the generation of radicals in the second stage, consequently increasing both conversion rates and energy efficiency despite the constant total plasma energy input. Another contributing factor to the performance improvement is that a larger, more homogeneous gas volume is exposed to the pulsed discharge in the second plasma stage, which can lead to an increased effective gas residence time within the plasma.
{"title":"Boosting CO₂ utilization in dry methane reforming using a two-stage DC-pulsed spark cold plasma reactor","authors":"P. Majidi , S. Jafarmadar , S. Fathi","doi":"10.1016/j.jcou.2026.103343","DOIUrl":"10.1016/j.jcou.2026.103343","url":null,"abstract":"<div><div>The dry methane reforming process holds the potential to convert the greenhouse gas carbon dioxide into high-value-added fuels and chemicals, presenting broad application prospects in the fields of environmental protection and renewable energy. In this study, a two-stage pulsed discharge cold plasma reactor was experimentally investigated at ambient temperature and atmospheric pressure. The primary products of this process were syngas (CO and H₂), with smaller quantities of C₂Hᵧ compounds (y = 2, 4, or 6) also produced as by-products. This research aims to examine and compare a single-stage plasma system with a two-stage system. The results demonstrate that a significant improvement in methane conversion and hydrogen selectivity is achieved when the plasma energy is discharged across two stages. This performance enhancement is attributed to the presence of hydrogen generated in the second plasma stage. These findings indicate that plasma power alone is not the sole factor determining optimal performance; rather, the method of its delivery can profoundly influence the conversion of methane and carbon dioxide, product yields, and energy conversion efficiency. In this configuration, the hydrogen produced in the first stage promotes the generation of radicals in the second stage, consequently increasing both conversion rates and energy efficiency despite the constant total plasma energy input. Another contributing factor to the performance improvement is that a larger, more homogeneous gas volume is exposed to the pulsed discharge in the second plasma stage, which can lead to an increased effective gas residence time within the plasma.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103343"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-01-19DOI: 10.1016/j.jcou.2026.103332
Shiwen Ji , Youcheng Zheng , Youquan Liu , Ruoyu Yang , Yan Zhang , Yuehan Wei
The technology of switching to CO2 in natural gas reservoirs to enhance natural gas recovery is highly recognized for its ability to store carbon dioxide and improve gas recovery rates. However, the application of this technology in carbonate reservoirs with edge and bottom water presents two main challenges: the significant heterogeneity of carbonate rocks and the pronounced intrusion of edge and bottom water. This study investigates the mechanisms of Enhanced Gas Recovery and the basic laws of gas-water seepage in reservoirs through laboratory physical simulation experiments. Using core samples with varying permeability, high and low permeability conditions were simulated to characterize the heterogeneity of carbonate reservoirs. The experimental results indicate that: 1. After switching to CO2, high-permeability cores have better energy replenishment effects compared to low-permeability cores, with the recovery rate of high-permeability cores improving by 8.2 % compared to low-permeability cores; 2. The injected carbon dioxide can effectively push back the formation water that has intruded into both high and low permeability cores, releasing natural gas that was previously trapped by the formation water, thus alleviating the adverse effects of water intrusion that lead to low recovery rates; 3. Under different injection pressures, the recovery degree of high-permeability cores is consistently higher than that of low-permeability cores; when the pressure recovers to 100 %, the recovery rate of high-permeability cores reaches its highest level at 76.97 %, which is 30.79 % higher than that of low-permeability cores. Therefore, CO2-EGR technology demonstrates significant potential in controlling water intrusion and improving recovery efficiency in carbonate gas reservoirs.
{"title":"Study on enhancing natural gas recovery by CO2 injection in water-bearing heterogeneous carbonate reservoirs","authors":"Shiwen Ji , Youcheng Zheng , Youquan Liu , Ruoyu Yang , Yan Zhang , Yuehan Wei","doi":"10.1016/j.jcou.2026.103332","DOIUrl":"10.1016/j.jcou.2026.103332","url":null,"abstract":"<div><div>The technology of switching to CO<sub>2</sub> in natural gas reservoirs to enhance natural gas recovery is highly recognized for its ability to store carbon dioxide and improve gas recovery rates. However, the application of this technology in carbonate reservoirs with edge and bottom water presents two main challenges: the significant heterogeneity of carbonate rocks and the pronounced intrusion of edge and bottom water. This study investigates the mechanisms of Enhanced Gas Recovery and the basic laws of gas-water seepage in reservoirs through laboratory physical simulation experiments. Using core samples with varying permeability, high and low permeability conditions were simulated to characterize the heterogeneity of carbonate reservoirs. The experimental results indicate that: 1. After switching to CO<sub>2</sub>, high-permeability cores have better energy replenishment effects compared to low-permeability cores, with the recovery rate of high-permeability cores improving by 8.2 % compared to low-permeability cores; 2. The injected carbon dioxide can effectively push back the formation water that has intruded into both high and low permeability cores, releasing natural gas that was previously trapped by the formation water, thus alleviating the adverse effects of water intrusion that lead to low recovery rates; 3. Under different injection pressures, the recovery degree of high-permeability cores is consistently higher than that of low-permeability cores; when the pressure recovers to 100 %, the recovery rate of high-permeability cores reaches its highest level at 76.97 %, which is 30.79 % higher than that of low-permeability cores. Therefore, CO<sub>2</sub>-EGR technology demonstrates significant potential in controlling water intrusion and improving recovery efficiency in carbonate gas reservoirs.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103332"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025235","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-01-16DOI: 10.1016/j.jcou.2026.103330
Jia-Ying Sie , Tzu-Hung Wen , Po-Yang Peng , Ying-Rui Lu , Chi-Liang Chen , Yu-Chuan Lin
Nickel catalysts supported on silica were synthesized via a molten salt method (MSM) using Na- and K-based salts with Cl⁻ or Br⁻ counterions, and evaluated in low-temperature reverse water–gas shift (RWGS) reaction. Despite similar Ni nanoparticle sizes, the presence of residual salts significantly influenced catalyst performance by altering the electronic properties of Ni and the nature of surface carbonates. X-ray absorption spectroscopy (XAS) revealed negatively charged Ni species (Niδ⁻), particularly in Br-containing samples. H2-temperature programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS) confirmed Ni-Cl and Ni-Br interactions, and the latter showed a higher extent. In-situ infrared studies indicated that Br-based catalysts suppressed the formation of bidentate carbonate (b-*CO3), a spectator that passivates active sites, and instead favored monodentate carbonate (m-*CO3), leading to higher CO2 conversions. The r-Ni@Na1.9K3.3Br(5)/SiO2 catalyst achieved stable CO2 conversion (ca. 35 %) with 100 % CO selectivity and 100-hour durability. These results highlight the importance of halide identity in modulating Ni–salt interactions and reaction pathways for RWGS.
{"title":"Silica-supported nickel catalysts synthesized via the molten salt method for reverse water-gas shift: Impact of chlorine and bromine halides","authors":"Jia-Ying Sie , Tzu-Hung Wen , Po-Yang Peng , Ying-Rui Lu , Chi-Liang Chen , Yu-Chuan Lin","doi":"10.1016/j.jcou.2026.103330","DOIUrl":"10.1016/j.jcou.2026.103330","url":null,"abstract":"<div><div>Nickel catalysts supported on silica were synthesized via a molten salt method (MSM) using Na- and K-based salts with Cl⁻ or Br⁻ counterions, and evaluated in low-temperature reverse water–gas shift (RWGS) reaction. Despite similar Ni nanoparticle sizes, the presence of residual salts significantly influenced catalyst performance by altering the electronic properties of Ni and the nature of surface carbonates. X-ray absorption spectroscopy (XAS) revealed negatively charged Ni species (Ni<sup>δ⁻</sup>), particularly in Br-containing samples. H<sub>2</sub>-temperature programmed reduction (TPR) and X-ray photoelectron spectroscopy (XPS) confirmed Ni-Cl and Ni-Br interactions, and the latter showed a higher extent. In-situ infrared studies indicated that Br-based catalysts suppressed the formation of bidentate carbonate (b-*CO<sub>3</sub>), a spectator that passivates active sites, and instead favored monodentate carbonate (m-*CO<sub>3</sub>), leading to higher CO<sub>2</sub> conversions. The r-Ni@Na<sub>1.9</sub>K<sub>3.3</sub>Br(5)/SiO<sub>2</sub> catalyst achieved stable CO<sub>2</sub> conversion (<em>ca.</em> 35 %) with 100 % CO selectivity and 100-hour durability. These results highlight the importance of halide identity in modulating Ni–salt interactions and reaction pathways for RWGS.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103330"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145976258","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-02-09DOI: 10.1016/j.jcou.2026.103338
Rohan Sartape , Rohit Chauhan , Samdavid Swaminathan , Ishita Goyal , Amey Thorat , Jindal K. Shah , Meenesh R. Singh
Carbon capture and storage (CCS) plays a critical role in achieving climate change mitigation targets, offering a pathway to decarbonize power generation, industrial processes, and heat production while addressing atmospheric CO2 removal. While CCS technologies are technically advanced, the widespread adoption of 100 % CO2 capture capacities such as 1 mol of CO2/mol of material and 1 g CO2/g storage (targeted by the DARPA, Defense Sciences Office, USA Govt.) has raised questions about the feasibility of achieving higher capture capacities. In the context of limiting global warming to 1.5°C, reaching 100 % CO2 capture capacity is increasingly necessary, with residual emissions requiring complementary carbon dioxide removal (CDR) technologies. This review exclusively focuses on the CO2 capture capacities of various sorbents under standard conditions, using different evaluation metrics. This study explores the performance of solid and liquid sorbents under standard conditions, analyzing factors including surface area, pore structure, solvent type, and functionalization to identify materials optimized for industrial-scale CCS applications. Emerging sorbents, including ILs, MOFs, COFs, POPs, DES, RCC, hybrid materials, and reactive sorbents, offer significant potential for enhanced selectivity and energy-efficient regeneration. Through a systematic assessment of gravimetric, volumetric, and molar capacities, the study provides insights into material efficiencies and trade-offs, offering guidance on optimizing sorbent selection for specific applications. The research advances understanding of scalable CCS technologies, contributing to global efforts to achieve net-zero emissions and address the pressing challenge of climate change.
碳捕集与封存（CCS）在实现减缓气候变化目标方面发挥着关键作用，为发电、工业过程和产热脱碳提供了一条途径，同时解决了大气中二氧化碳的去除问题。虽然CCS技术在技术上是先进的，但广泛采用100% %的二氧化碳捕获能力，如1 mol CO2/mol材料和1 g CO2/g存储（美国国防部高级研究计划局，国防科学办公室，美国政府的目标），已经提出了关于实现更高捕获能力可行性的问题。在将全球变暖限制在1.5°C的背景下，越来越有必要达到100% %的二氧化碳捕获能力，剩余排放需要补充二氧化碳去除（CDR）技术。本文主要介绍了不同吸附剂在标准条件下的CO2捕集能力，采用不同的评价指标。本研究探讨了固体和液体吸附剂在标准条件下的性能，分析了表面积、孔隙结构、溶剂类型和功能化等因素，以确定适合工业规模CCS应用的优化材料。新兴的吸附剂，包括ILs、mof、COFs、POPs、DES、RCC、杂化材料和反应性吸附剂，在提高选择性和节能再生方面具有巨大的潜力。通过对重量、体积和摩尔容量的系统评估，该研究提供了对材料效率和权衡的见解，为优化特定应用的吸附剂选择提供了指导。这项研究促进了对可扩展的CCS技术的理解，为全球实现净零排放和应对气候变化的紧迫挑战做出了贡献。
{"title":"Trends and limits of CO2 capture in solid and liquid sorbents at standard conditions","authors":"Rohan Sartape , Rohit Chauhan , Samdavid Swaminathan , Ishita Goyal , Amey Thorat , Jindal K. Shah , Meenesh R. Singh","doi":"10.1016/j.jcou.2026.103338","DOIUrl":"10.1016/j.jcou.2026.103338","url":null,"abstract":"<div><div>Carbon capture and storage (CCS) plays a critical role in achieving climate change mitigation targets, offering a pathway to decarbonize power generation, industrial processes, and heat production while addressing atmospheric CO<sub>2</sub> removal. While CCS technologies are technically advanced, the widespread adoption of 100 % CO<sub>2</sub> capture capacities such as 1 mol of CO<sub>2</sub>/mol of material and 1 g CO<sub>2</sub>/g storage (targeted by the DARPA, Defense Sciences Office, USA Govt.) has raised questions about the feasibility of achieving higher capture capacities. In the context of limiting global warming to 1.5°C, reaching 100 % CO<sub>2</sub> capture capacity is increasingly necessary, with residual emissions requiring complementary carbon dioxide removal (CDR) technologies. This review exclusively focuses on the CO<sub>2</sub> capture capacities of various sorbents under standard conditions, using different evaluation metrics. This study explores the performance of solid and liquid sorbents under standard conditions, analyzing factors including surface area, pore structure, solvent type, and functionalization to identify materials optimized for industrial-scale CCS applications. Emerging sorbents, including ILs, MOFs, COFs, POPs, DES, RCC, hybrid materials, and reactive sorbents, offer significant potential for enhanced selectivity and energy-efficient regeneration. Through a systematic assessment of gravimetric, volumetric, and molar capacities, the study provides insights into material efficiencies and trade-offs, offering guidance on optimizing sorbent selection for specific applications. The research advances understanding of scalable CCS technologies, contributing to global efforts to achieve net-zero emissions and address the pressing challenge of climate change.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103338"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170705","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-02-03DOI: 10.1016/j.jcou.2026.103347
Samuel Jaro Kaufmann, Joe Quade, Johanna Buschmann, Haripriya Chinnaraj, Kai Peter Birke, Paul Rößner
In this work, we investigated large-volume, non-thermal discharges in CO₂/CH₄ mixtures with the aim of enabling energy-efficient plasma-based conversion. Building on the fundamental U–I characteristics of gas discharges, we showed how discharge extension and thermal management strongly affect the transition between glow and arc regimes. Using our Big Discharge-gap Glow-to-Arc (BDGTA) reactor, stable rotating discharges were realized at electrode gaps up to 40 mm. Depending on scale, plasma operation was achieved with average currents of 0.24–0.4 A and discharge voltages ranging from 1.5 kV (15 mm) to 4 kV (40 mm), corresponding to power levels between 400 and 1700 W. Optical diagnostics via high-speed camera confirmed the glow-like nature and the dynamics of the elongated discharges. Performance analysis revealed maximum energy efficiencies of 68 % (60 % CO2, 40 % CH4) and 60 % for 50/50 mixtures, with conversions up to 68 %. Carbon deposition in methane-rich mixtures was identified as a key challenge but can be mitigated through process adjustments like CO₂ recycling. Replacing ballast resistors with power-electronics plasma control minimized energy losses and ensured regime stability. Overall, the BDGTA reactor demonstrates that efficient, large-volume CO₂/CH₄ plasma conversion is feasible at atmospheric pressure, offering a pathway for sustainable electrification of chemical processes.
{"title":"CO2 and CH4 conversion in a rotating DC glow to arc plasma with big discharge gap","authors":"Samuel Jaro Kaufmann, Joe Quade, Johanna Buschmann, Haripriya Chinnaraj, Kai Peter Birke, Paul Rößner","doi":"10.1016/j.jcou.2026.103347","DOIUrl":"10.1016/j.jcou.2026.103347","url":null,"abstract":"<div><div>In this work, we investigated large-volume, non-thermal discharges in CO₂/CH₄ mixtures with the aim of enabling energy-efficient plasma-based conversion. Building on the fundamental U–I characteristics of gas discharges, we showed how discharge extension and thermal management strongly affect the transition between glow and arc regimes. Using our Big Discharge-gap Glow-to-Arc (BDGTA) reactor, stable rotating discharges were realized at electrode gaps up to 40 mm. Depending on scale, plasma operation was achieved with average currents of 0.24–0.4 A and discharge voltages ranging from 1.5 kV (15 mm) to 4 kV (40 mm), corresponding to power levels between 400 and 1700 W. Optical diagnostics via high-speed camera confirmed the glow-like nature and the dynamics of the elongated discharges. Performance analysis revealed maximum energy efficiencies of 68 % (60 % CO<sub>2</sub>, 40 % CH<sub>4</sub>) and 60 % for 50/50 mixtures, with conversions up to 68 %. Carbon deposition in methane-rich mixtures was identified as a key challenge but can be mitigated through process adjustments like CO₂ recycling. Replacing ballast resistors with power-electronics plasma control minimized energy losses and ensured regime stability. Overall, the BDGTA reactor demonstrates that efficient, large-volume CO₂/CH₄ plasma conversion is feasible at atmospheric pressure, offering a pathway for sustainable electrification of chemical processes.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103347"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146170709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-01-17DOI: 10.1016/j.jcou.2026.103313
Beatrice Senoner , Andrea Osti , Davide Chinello , Giovanni Agostini , Antonella Glisenti
In the scenario of climate change, dry reforming of methane (DRM) is a well-studied reaction where CO2 and CH4 are converted into syngas, a mixture composed of CO and H2 widely used in industries. However, DRM industrialization is hindered by the high operating temperatures and catalyst deactivation, mainly due to coking - i.e., carbon deposition. This work aims to mitigate the coking problem by alternating DRM with a NO flux which gasifies carbon above 677 °C into CO/CO2. Three Ni-impregnated catalysts are designed for this dual process: the chosen supports are γ-Al2O3, for its high dispersion and strong interaction with Ni, LaFeO3, for its NOx abatement properties and a mixed support LaFeO3-Al2O3. Only by combining the support properties in Ni/LaFeO3-Al2O3 catalyst nickel particles can be protected by NO oxidation, allowing increased conversions after NO flux and highlighting the need of combining catalyst and process design to achieve efficient and synergical pollutants abatement.
{"title":"Coupling DRM and NO reduction: A catalyst design strategy to control coking in Ni-based catalysts","authors":"Beatrice Senoner , Andrea Osti , Davide Chinello , Giovanni Agostini , Antonella Glisenti","doi":"10.1016/j.jcou.2026.103313","DOIUrl":"10.1016/j.jcou.2026.103313","url":null,"abstract":"<div><div>In the scenario of climate change, dry reforming of methane (DRM) is a well-studied reaction where CO<sub>2</sub> and CH<sub>4</sub> are converted into syngas, a mixture composed of CO and H<sub>2</sub> widely used in industries. However, DRM industrialization is hindered by the high operating temperatures and catalyst deactivation, mainly due to coking - i.e., carbon deposition. This work aims to mitigate the coking problem by alternating DRM with a NO flux which gasifies carbon above 677 °C into CO/CO<sub>2</sub>. Three Ni-impregnated catalysts are designed for this dual process: the chosen supports are γ-Al<sub>2</sub>O<sub>3</sub>, for its high dispersion and strong interaction with Ni, LaFeO<sub>3</sub>, for its NOx abatement properties and a mixed support LaFeO<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub>. Only by combining the support properties in Ni/LaFeO<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub> catalyst nickel particles can be protected by NO oxidation, allowing increased conversions after NO flux and highlighting the need of combining catalyst and process design to achieve efficient and synergical pollutants abatement.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103313"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145976257","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2026-01-16DOI: 10.1016/j.jcou.2026.103327
Dahi Akmach , Shang Jiang , Anik Ashirwadam , Malak El Kaddouri , Samir H. Mushrif , Serge Kaliaguine , David S.A. Simakov
For the sustainable utilization of carbon dioxide (CO2), the development of an inexpensive, active, selective and highly stable catalyst is essential to overcome the economic challenges in its reduction to carbon monoxide (CO). Molybdenum and tungsten carbides-based materials are regarded as attractive catalysts for the reverse water gas shift RWGS reaction. This work began with a series of catalytic tests indicating that mixed Mo-W carbides behave essentially like blends of monocarbides Mo2C and WC. To establish a performance baseline, an in-depth evaluation of the two monometallic carbides was conducted enabling a precise assessment of their intrinsic activity and mechanistic behavior under RWGS conditions. The results revealed that Mo2C promoted the formation of both CH4 and CO, while increasing the tungsten content gradually, enhances CO selectivity with decreasing reaction rate. Monometallic tungsten carbide WC achieved complete CO selectivity and maintained it even after 100 h exposure to harsh reaction conditions at 600 ˚C. In-situ DRIFTS and density functional theory (DFT) calculations revealed that WC can achieve 100 % CO selectivity through two distinct mechanisms on different facets, a concerted redox mechanism on WC (-100), and an associative mechanism on WC (101) facet where further hydrogenation of *CHO intermediate is kinetically unfavorable. Both pathways steer the reaction toward CO production and prevent the formation of undesired side product CH4. This work not only provides valuable insights into the role of metal carbide phases in catalytic performance but also contributes to the fundamental understanding of reaction mechanism.
{"title":"Molybdenum and tungsten carbides as catalysts for the reverse water gas shift reaction","authors":"Dahi Akmach , Shang Jiang , Anik Ashirwadam , Malak El Kaddouri , Samir H. Mushrif , Serge Kaliaguine , David S.A. Simakov","doi":"10.1016/j.jcou.2026.103327","DOIUrl":"10.1016/j.jcou.2026.103327","url":null,"abstract":"<div><div>For the sustainable utilization of carbon dioxide (CO<sub>2</sub>), the development of an inexpensive, active, selective and highly stable catalyst is essential to overcome the economic challenges in its reduction to carbon monoxide (CO). Molybdenum and tungsten carbides-based materials are regarded as attractive catalysts for the reverse water gas shift RWGS reaction. This work began with a series of catalytic tests indicating that mixed Mo-W carbides behave essentially like blends of monocarbides Mo<sub>2</sub>C and WC. To establish a performance baseline, an in-depth evaluation of the two monometallic carbides was conducted enabling a precise assessment of their intrinsic activity and mechanistic behavior under RWGS conditions. The results revealed that Mo<sub>2</sub>C promoted the formation of both CH<sub>4</sub> and CO, while increasing the tungsten content gradually, enhances CO selectivity with decreasing reaction rate. Monometallic tungsten carbide WC achieved complete CO selectivity and maintained it even after 100 h exposure to harsh reaction conditions at 600 ˚C. In-situ DRIFTS and density functional theory (DFT) calculations revealed that WC can achieve 100 % CO selectivity through two distinct mechanisms on different facets, a concerted redox mechanism on WC (-100), and an associative mechanism on WC (101) facet where further hydrogenation of *CHO intermediate is kinetically unfavorable. Both pathways steer the reaction toward CO production and prevent the formation of undesired side product CH<sub>4</sub>. This work not only provides valuable insights into the role of metal carbide phases in catalytic performance but also contributes to the fundamental understanding of reaction mechanism.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"105 ","pages":"Article 103327"},"PeriodicalIF":8.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145976259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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