Pub Date : 2025-02-01DOI: 10.1016/j.jcou.2025.103022
Kairi Yamamoto, Ikuo Ushiki
Ibuprofen and ketoprofen were impregnated onto SBA-15 type mesoporous silica using the supercritical fluid deposition (SCFD) method with supercritical carbon dioxide (CO2) as the solvent at temperatures ranging from 313 K to 343 K and a pressure of 15 MPa. The prepared samples were evaluated using electron microscopy, nitrogen adsorption measurements, infrared spectroscopy, and thermogravimetric analysis. The impregnation of the drugs into the mesoporous silica pores was confirmed by nitrogen adsorption experiments. The amount of drug impregnation was found to depend on both the drug species and the type of mesoporous silica. It was suggested that the solubility in supercritical CO2 played a dominant role for the drug species. There was virtually no effect of temperature on the amount of drug impregnation, which may be attributed to the interplay between the solubility of supercritical CO2 and the adsorption equilibrium of the drug on mesoporous silica under supercritical CO2 conditions.
{"title":"Impregnation of non-steroidal anti-inflammatory drugs (ibuprofen and ketoprofen) onto mesoporous silica SBA-15 using supercritical CO2","authors":"Kairi Yamamoto, Ikuo Ushiki","doi":"10.1016/j.jcou.2025.103022","DOIUrl":"10.1016/j.jcou.2025.103022","url":null,"abstract":"<div><div>Ibuprofen and ketoprofen were impregnated onto SBA-15 type mesoporous silica using the supercritical fluid deposition (SCFD) method with supercritical carbon dioxide (CO<sub>2</sub>) as the solvent at temperatures ranging from 313 K to 343 K and a pressure of 15 MPa. The prepared samples were evaluated using electron microscopy, nitrogen adsorption measurements, infrared spectroscopy, and thermogravimetric analysis. The impregnation of the drugs into the mesoporous silica pores was confirmed by nitrogen adsorption experiments. The amount of drug impregnation was found to depend on both the drug species and the type of mesoporous silica. It was suggested that the solubility in supercritical CO<sub>2</sub> played a dominant role for the drug species. There was virtually no effect of temperature on the amount of drug impregnation, which may be attributed to the interplay between the solubility of supercritical CO<sub>2</sub> and the adsorption equilibrium of the drug on mesoporous silica under supercritical CO<sub>2</sub> conditions.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"92 ","pages":"Article 103022"},"PeriodicalIF":7.2,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143182652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.jcou.2025.103021
Farag M.A. Altalbawy , Nadhir N.A. Jafar , Dharmesh Sur , Anupam Yadav , Subbulakshmi Ganesan , Aman Shankhyan , M. Ravi Kumar , Girish Chandra Sharma , Iskandar Shernazarov , Sarah Qutayba Badraldin , Uday Abdul-Reda Hussein , Khursheed Muzammil , Hossein Mahabadi Asl
The current study aims at modeling the solubility of anti-cancer agents in supercritical carbon dioxide (SC-CO2). An extensive databank, including 893 measured samples for 33 anti-cancer agents were collected from the literature, covering extensive ranges of operating conditions. Eight density-based empirical models were firstly employed to correlate the collected data. After adjusting their constant coefficients, four of them provided satisfactory estimations, with total average absolute relative errors (AAREs) below 10 %. A novel six-parameter empirical correlation was also proposed, with input factors optimized based on the Pearson coefficient analysis. This correlation produced satisfactory results for the analyzed drugs, achieving a total AARE of 7.71 %. Afterward, a generalized and unified model was built using the intelligent method of gaussian process regression (GPR). For the testing data, this model showed excellent results with AARE and R2 values of 2.90 % and 99.87 %, respectively. Furthermore, its estimations for all anti-cancer agents outperformed the empirical correlations significantly. Both empirical and intelligent models accurately described the physical behavior of anti-cancer agents’ solubility in SC-CO2 under various conditions. Subsequently, the most effective factors on the performances of the models were recognized through a sensitivity analysis.
{"title":"Universal data-driven models to estimate the solubility of anti-cancer drugs in supercritical carbon dioxide: Correlation development and machine learning modeling","authors":"Farag M.A. Altalbawy , Nadhir N.A. Jafar , Dharmesh Sur , Anupam Yadav , Subbulakshmi Ganesan , Aman Shankhyan , M. Ravi Kumar , Girish Chandra Sharma , Iskandar Shernazarov , Sarah Qutayba Badraldin , Uday Abdul-Reda Hussein , Khursheed Muzammil , Hossein Mahabadi Asl","doi":"10.1016/j.jcou.2025.103021","DOIUrl":"10.1016/j.jcou.2025.103021","url":null,"abstract":"<div><div>The current study aims at modeling the solubility of anti-cancer agents in supercritical carbon dioxide (SC-CO<sub>2</sub>). An extensive databank, including 893 measured samples for 33 anti-cancer agents were collected from the literature, covering extensive ranges of operating conditions. Eight density-based empirical models were firstly employed to correlate the collected data. After adjusting their constant coefficients, four of them provided satisfactory estimations, with total average absolute relative errors (AAREs) below 10 %. A novel six-parameter empirical correlation was also proposed, with input factors optimized based on the Pearson coefficient analysis. This correlation produced satisfactory results for the analyzed drugs, achieving a total AARE of 7.71 %. Afterward, a generalized and unified model was built using the intelligent method of gaussian process regression (GPR). For the testing data, this model showed excellent results with AARE and R<sup>2</sup> values of 2.90 % and 99.87 %, respectively. Furthermore, its estimations for all anti-cancer agents outperformed the empirical correlations significantly. Both empirical and intelligent models accurately described the physical behavior of anti-cancer agents’ solubility in SC-CO<sub>2</sub> under various conditions. Subsequently, the most effective factors on the performances of the models were recognized through a sensitivity analysis.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"92 ","pages":"Article 103021"},"PeriodicalIF":7.2,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143182651","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The hydrogenation of bicarbonates in aqueous solutions using a Pd-based catalyst is an effective method for the production of formate. Herein, we synthesized finely dispersed Pd/CeO2 catalysts via a two-step calcination method and evaluated their catalytic activities before and after the reduction process. The unreduced Pd/CeO2 catalyst exhibited significantly higher activity for bicarbonate hydrogenation than the reduced catalyst. Although the activity declined after multiple cycles, regeneration via calcination effectively restored activity by converting metallic Pd back to highly active PdO. In addition, Pd incorporation and reaction conditions increased Ce3 + contents and oxygen vacancies in CeO2, enhancing bicarbonate adsorption and catalytic performance. These findings highlight the roles of PdO and oxygen vacancies in the CeO2 support in the catalytic activity of Pd/CeO2 catalysts for bicarbonate hydrogenation.
{"title":"Exploring the role of PdO and oxygen vacancies of Pd/CeO2 in bicarbonate hydrogenation","authors":"Hyun-Wook Jeong , Gwang-Nam Yun , Youn-Sang Bae , Kyung-Ryul Oh , Young Kyu Hwang","doi":"10.1016/j.jcou.2025.103028","DOIUrl":"10.1016/j.jcou.2025.103028","url":null,"abstract":"<div><div>The hydrogenation of bicarbonates in aqueous solutions using a Pd-based catalyst is an effective method for the production of formate. Herein, we synthesized finely dispersed Pd/CeO<sub>2</sub> catalysts via a two-step calcination method and evaluated their catalytic activities before and after the reduction process. The unreduced Pd/CeO<sub>2</sub> catalyst exhibited significantly higher activity for bicarbonate hydrogenation than the reduced catalyst. Although the activity declined after multiple cycles, regeneration via calcination effectively restored activity by converting metallic Pd back to highly active PdO. In addition, Pd incorporation and reaction conditions increased Ce<sup>3 +</sup> contents and oxygen vacancies in CeO<sub>2</sub>, enhancing bicarbonate adsorption and catalytic performance. These findings highlight the roles of PdO and oxygen vacancies in the CeO<sub>2</sub> support in the catalytic activity of Pd/CeO<sub>2</sub> catalysts for bicarbonate hydrogenation.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"92 ","pages":"Article 103028"},"PeriodicalIF":7.2,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143182609","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.jcou.2024.103014
Song He , Lifan Gao , Yawen Zheng , Junyao Wang , Shenghui Lin , Zhi Yang , Xuelan Zeng
Calcium looping process has presented great potential realizing low-energy-consumption CO2 capture since high-grade thermal energy can be recovered. However, in current calcium looping configurations, the carbonation heat is recovered for steam generation, resulting in the significant exergy destruction. This study presents a novel Ca-Cu looping process with thermochemical recuperation to address the significant exergy destruction during carbonation heat recovery. System integration is carried out for the typical flue gas decarbonization. Results indicate that the proposed system present superior performance than that in the reference system without thermochemical recuperation. The specific primary energy consumption for CO2 avoided decreases from 2.29 MJLHV/kg CO2 in the reference system to 1.68 MJLHV/kg CO2 in the proposed system. Energy analysis and exergy analysis reveal that carbonation heat recovery via thermochemical recuperation and efficient utilization of the increased chemical energy contribute to reduction of energy consumption. The research also examines how operating conditions impact the thermodynamic efficiency. An optimized primary energy consumption for CO2 avoidance of 1.58 MJLHV/kg CO2 can be achieved through the response surface method. Besides, the cost of CO2 avoided can achieved at 37.52 €/t CO2, which is more economically feasible with that of the conventional calcium looping technology.
{"title":"Carbonation heat recovery via dry reforming to improve the techno-economic performance of the Ca-Cu looping post-combustion CO2 capture","authors":"Song He , Lifan Gao , Yawen Zheng , Junyao Wang , Shenghui Lin , Zhi Yang , Xuelan Zeng","doi":"10.1016/j.jcou.2024.103014","DOIUrl":"10.1016/j.jcou.2024.103014","url":null,"abstract":"<div><div>Calcium looping process has presented great potential realizing low-energy-consumption CO<sub>2</sub> capture since high-grade thermal energy can be recovered. However, in current calcium looping configurations, the carbonation heat is recovered for steam generation, resulting in the significant exergy destruction. This study presents a novel Ca-Cu looping process with thermochemical recuperation to address the significant exergy destruction during carbonation heat recovery. System integration is carried out for the typical flue gas decarbonization. Results indicate that the proposed system present superior performance than that in the reference system without thermochemical recuperation. The specific primary energy consumption for CO<sub>2</sub> avoided decreases from 2.29 MJ<sub>LHV</sub>/kg CO<sub>2</sub> in the reference system to 1.68 MJ<sub>LHV</sub>/kg CO<sub>2</sub> in the proposed system. Energy analysis and exergy analysis reveal that carbonation heat recovery via thermochemical recuperation and efficient utilization of the increased chemical energy contribute to reduction of energy consumption. The research also examines how operating conditions impact the thermodynamic efficiency. An optimized primary energy consumption for CO<sub>2</sub> avoidance of 1.58 MJ<sub>LHV</sub>/kg CO<sub>2</sub> can be achieved through the response surface method. Besides, the cost of CO<sub>2</sub> avoided can achieved at 37.52 €/t CO<sub>2</sub>, which is more economically feasible with that of the conventional calcium looping technology.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"92 ","pages":"Article 103014"},"PeriodicalIF":7.2,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143182714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.jcou.2024.103001
Yasemen Kuddusi , Laura Piveteau , Mounir Mensi , Daniel C. Cano-Blanco , Andreas Züttel
Direct light olefin synthesis from CO2 hydrogenation is a new pathway to decarbonize the chemical industry. Inspired by the promising catalytic activity of Ga2O3-based catalysts in alkane dehydrogenation, this study reveals that optimizing Ga content in the GaxIn2-xO3/SSZ-13 catalytic system can narrow the product distribution toward light olefins. The optimized catalyst exhibits light olefin and C2H4 selectivity up to 84 % and 45.9 %, respectively, amongst C2+ hydrocarbons with a maximum olefin/paraffin ratio of 6.4 and a CO2 conversion of 14.8 % at 20 bar and 653 K. In particular, a sevenfold increase in C2H4 space-time yield compared to pure metal oxides on SSZ-13 was observed, along with the gradual suppression of C3H8 formation. Herein, we established a catalyst structure-performance relationship as a function of chemical composition. As such, CO and paraffin formation rates can be suppressed, and light olefin formation rates can be enhanced. Therefore, the change in light olefin STY upon gallium incorporation could be ascribed to modulations in the structural and electronic properties, as well as alterations in the surface adsorption and acidic strengths. The findings presented here provide a strategy to tune CO2 hydrogenation product distributions toward specific target products.
{"title":"Selective light olefin synthesis with high ethylene abundance via CO2 hydrogenation over (Ga-In)2O3/SSZ-13 catalysts","authors":"Yasemen Kuddusi , Laura Piveteau , Mounir Mensi , Daniel C. Cano-Blanco , Andreas Züttel","doi":"10.1016/j.jcou.2024.103001","DOIUrl":"10.1016/j.jcou.2024.103001","url":null,"abstract":"<div><div>Direct light olefin synthesis from CO<sub>2</sub> hydrogenation is a new pathway to decarbonize the chemical industry. Inspired by the promising catalytic activity of Ga<sub>2</sub>O<sub>3</sub>-based catalysts in alkane dehydrogenation, this study reveals that optimizing Ga content in the Ga<sub>x</sub>In<sub>2-x</sub>O<sub>3</sub>/SSZ-13 catalytic system can narrow the product distribution toward light olefins. The optimized catalyst exhibits light olefin and C<sub>2</sub>H<sub>4</sub> selectivity up to 84 % and 45.9 %, respectively, amongst C<sub>2+</sub> hydrocarbons with a maximum olefin/paraffin ratio of 6.4 and a CO<sub>2</sub> conversion of 14.8 % at 20 bar and 653 K. In particular, a sevenfold increase in C<sub>2</sub>H<sub>4</sub> space-time yield compared to pure metal oxides on SSZ-13 was observed, along with the gradual suppression of C<sub>3</sub>H<sub>8</sub> formation. Herein, we established a catalyst structure-performance relationship as a function of chemical composition. As such, CO and paraffin formation rates can be suppressed, and light olefin formation rates can be enhanced. Therefore, the change in light olefin STY upon gallium incorporation could be ascribed to modulations in the structural and electronic properties, as well as alterations in the surface adsorption and acidic strengths. The findings presented here provide a strategy to tune CO<sub>2</sub> hydrogenation product distributions toward specific target products.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"91 ","pages":"Article 103001"},"PeriodicalIF":7.2,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143178104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.jcou.2024.103006
Weihao Li , Jiapeng Yang , Ming Sun , Fengxia Xu , Yan Zhao , Handuo Xia
Foam concrete, as a common road fill material, has long been widely studied. This paper examined the compressive strength, water absorption rate, freeze-thaw resistance, Young's modulus, erosion resistance, and thermal conductivity of foam concrete with various densities and sludge contents. SEM and XRD images were utilized to study the impact of different sludge levels on hydration products. Environmental impacts were analyzed using life cycle assessment, and the optimal mix ratios were determined using the TOPSIS method. Results showed that incorporating a small amount of sludge (10 %) does not significantly impact the performance of foam concrete and can even slightly enhance compressive strength at a density of 800 kg/m3. The addition of sludge altered the internal pore structure, reduced thermal conductivity, decreased freeze-thaw resistance and Young's modulus, but improved erosion resistance and promoted the formation of AFt and AFm. Foam concrete with a density of 800 kg/m3 and 10 % sludge content exhibited the best overall performance. Substituting sludge for cement in foam concrete production effectively reduces carbon emissions.
{"title":"A sludge-modified foam concrete for road fill material: Performance evaluation and carbon footprint analysis","authors":"Weihao Li , Jiapeng Yang , Ming Sun , Fengxia Xu , Yan Zhao , Handuo Xia","doi":"10.1016/j.jcou.2024.103006","DOIUrl":"10.1016/j.jcou.2024.103006","url":null,"abstract":"<div><div>Foam concrete, as a common road fill material, has long been widely studied. This paper examined the compressive strength, water absorption rate, freeze-thaw resistance, Young's modulus, erosion resistance, and thermal conductivity of foam concrete with various densities and sludge contents. SEM and XRD images were utilized to study the impact of different sludge levels on hydration products. Environmental impacts were analyzed using life cycle assessment, and the optimal mix ratios were determined using the TOPSIS method. Results showed that incorporating a small amount of sludge (10 %) does not significantly impact the performance of foam concrete and can even slightly enhance compressive strength at a density of 800 kg/m<sup>3</sup>. The addition of sludge altered the internal pore structure, reduced thermal conductivity, decreased freeze-thaw resistance and Young's modulus, but improved erosion resistance and promoted the formation of AFt and AFm. Foam concrete with a density of 800 kg/m<sup>3</sup> and 10 % sludge content exhibited the best overall performance. Substituting sludge for cement in foam concrete production effectively reduces carbon emissions.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"91 ","pages":"Article 103006"},"PeriodicalIF":7.2,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143176987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.jcou.2024.102999
Yiming Wang , Wensheng Wei , Yuxin Wang , Guangwen Xu , Jinggang Zhao , Lei Shi
In this study, a series of hydroxy-functionalized quaternary ammonium salt catalysts, i.e., NEt3(HE)Br, NEt2(HE)2Br, NEt1(HE)3Br, and N(HE)4Br, were successfully prepared by quantitatively grafting hydrogen-bond donors (HBDs) as electrophilic sites on quaternary ammonium salts and then used to catalyze the cycloaddition of propylene oxide (PO) and carbon dioxide (CO2). The aim was to reveal the effects of different amounts of hydroxy-functionalized quaternary ammonium salts on their catalytic activities. The synergistic catalytic effect of NEt3(HE)Br and a biomass-based catalytic system (NEt3(HE)Br/Bio) on the cycloaddition reaction was systematically studied, and the influence mechanism of hydroxy-rich biomass on the cycloaddition reaction was elucidated. The promoting effects of the hydroxyl-group content, position and connection structure in different alcohol additives on the CO2 cycloaddition reaction were further investigated and the results demonstrated that when the additive molecule contains an appropriate number of ortho-hydroxyl groups and these hydroxyl groups are connected to groups with strong electron-withdrawing ability and small steric hindrance, the cycloaddition efficiency between PO and CO₂ can be significantly enhanced. The reason is that these hydroxyl groups not only provide more hydrogen bonds, enhancing the intermolecular interactions, but also help to stabilize the transition state of the reaction. Notably, when 0.48 g of NEt3(HE)Br was mixed with 0.48 g of cellulose as HBDs to catalyze the cycloaddition reaction of CO2 and PO, PO conversion reached 99.34 % within 2 h, exceeding that obtained with the catalytic reaction system without HBDs. In addition, the NEt3(HE)Br/cellulose catalytic system was demonstrated to be universal for catalyzing the cycloaddition reaction of different epoxides and CO2. This article provides theoretical guidance and new inspirations for the efficient utilization of hydroxy-containing biomass materials in CO2 conversion.
{"title":"Promotion mechanism of hydroxyl groups in catalyzing CO2 cycloaddition","authors":"Yiming Wang , Wensheng Wei , Yuxin Wang , Guangwen Xu , Jinggang Zhao , Lei Shi","doi":"10.1016/j.jcou.2024.102999","DOIUrl":"10.1016/j.jcou.2024.102999","url":null,"abstract":"<div><div>In this study, a series of hydroxy-functionalized quaternary ammonium salt catalysts, i.e., NEt<sub>3</sub>(HE)Br, NEt<sub>2</sub>(HE)<sub>2</sub>Br, NEt<sub>1</sub>(HE)<sub>3</sub>Br, and N(HE)<sub>4</sub>Br, were successfully prepared by quantitatively grafting hydrogen-bond donors (HBDs) as electrophilic sites on quaternary ammonium salts and then used to catalyze the cycloaddition of propylene oxide (PO) and carbon dioxide (CO<sub>2</sub>). The aim was to reveal the effects of different amounts of hydroxy-functionalized quaternary ammonium salts on their catalytic activities. The synergistic catalytic effect of NEt<sub>3</sub>(HE)Br and a biomass-based catalytic system (NEt<sub>3</sub>(HE)Br/Bio) on the cycloaddition reaction was systematically studied, and the influence mechanism of hydroxy-rich biomass on the cycloaddition reaction was elucidated. The promoting effects of the hydroxyl-group content, position and connection structure in different alcohol additives on the CO<sub>2</sub> cycloaddition reaction were further investigated and the results demonstrated that when the additive molecule contains an appropriate number of ortho-hydroxyl groups and these hydroxyl groups are connected to groups with strong electron-withdrawing ability and small steric hindrance, the cycloaddition efficiency between PO and CO₂ can be significantly enhanced. The reason is that these hydroxyl groups not only provide more hydrogen bonds, enhancing the intermolecular interactions, but also help to stabilize the transition state of the reaction. Notably, when 0.48 g of NEt<sub>3</sub>(HE)Br was mixed with 0.48 g of cellulose as HBDs to catalyze the cycloaddition reaction of CO<sub>2</sub> and PO, PO conversion reached 99.34 % within 2 h, exceeding that obtained with the catalytic reaction system without HBDs. In addition, the NEt<sub>3</sub>(HE)Br/cellulose catalytic system was demonstrated to be universal for catalyzing the cycloaddition reaction of different epoxides and CO<sub>2</sub>. This article provides theoretical guidance and new inspirations for the efficient utilization of hydroxy-containing biomass materials in CO<sub>2</sub> conversion.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"91 ","pages":"Article 102999"},"PeriodicalIF":7.2,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143177104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.jcou.2024.103010
Zihao Song , Rui Chen , Tianyu Wang , Haoliang Wu
Reactive magnesium oxide (MgO) cement (RMC) presents a promising approach to reducing CO2 emissions and mitigating environmental impacts in cement production. Owing to its capacity to form a durable, high-strength matrix, RMC is particularly suitable for producing Engineered Cementitious Composites (ECC) with enhanced structural integrity. This study leveraged RMC’s high carbonation potential to assess its influence on the sustainability and mechanical performance of carbonated MgO-based ECC. Specifically, the effects of varying MgO content on mechanical properties, crack patterns, and microstructure were investigated across six mix designs, with MgO dosages ranging from 40 % to 70 % of the binder, under both standard and accelerated carbonation curing conditions. Results indicated that higher MgO dosages improved compressive and flexural strengths, with CM0.7 (70 % MgO) achieving a compressive strength increase from 30.02 MPa to 63.62 MPa over 28 days. Microstructural analyses via SEM-EDS and XRD revealed carbonation-induced densification, enhancing crack control and fiber-matrix bonding. The study concludes that increasing MgO content enhances both the sustainability and mechanical resilience of carbonated MgO-based ECC, though optimal dosing is necessary to balance strength gains with dimensional stability. These findings underscore the potential of carbonated MgO-based ECC as an environmentally favorable option for sustainable construction applications.
{"title":"Synergistic effects of CO2 sequestration on mechanical, microstructural, and environmental performance in carbonated MgO-based ECC","authors":"Zihao Song , Rui Chen , Tianyu Wang , Haoliang Wu","doi":"10.1016/j.jcou.2024.103010","DOIUrl":"10.1016/j.jcou.2024.103010","url":null,"abstract":"<div><div>Reactive magnesium oxide (MgO) cement (RMC) presents a promising approach to reducing CO<sub>2</sub> emissions and mitigating environmental impacts in cement production. Owing to its capacity to form a durable, high-strength matrix, RMC is particularly suitable for producing Engineered Cementitious Composites (ECC) with enhanced structural integrity. This study leveraged RMC’s high carbonation potential to assess its influence on the sustainability and mechanical performance of carbonated MgO-based ECC. Specifically, the effects of varying MgO content on mechanical properties, crack patterns, and microstructure were investigated across six mix designs, with MgO dosages ranging from 40 % to 70 % of the binder, under both standard and accelerated carbonation curing conditions. Results indicated that higher MgO dosages improved compressive and flexural strengths, with CM0.7 (70 % MgO) achieving a compressive strength increase from 30.02 MPa to 63.62 MPa over 28 days. Microstructural analyses via SEM-EDS and XRD revealed carbonation-induced densification, enhancing crack control and fiber-matrix bonding. The study concludes that increasing MgO content enhances both the sustainability and mechanical resilience of carbonated MgO-based ECC, though optimal dosing is necessary to balance strength gains with dimensional stability. These findings underscore the potential of carbonated MgO-based ECC as an environmentally favorable option for sustainable construction applications.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"91 ","pages":"Article 103010"},"PeriodicalIF":7.2,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143178102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.jcou.2024.103005
Wander Y. Perez-Sena , Fabrizio Ciccarelli , Kari Eränen , Martino Di Serio , Vincenzo Russo , Tapio Salmi
The conversion of CO2 into value-added cyclic carbonates via cycloaddition to bio-derived epoxides presents a sustainable approach for CO2 utilization. However, the production of cyclic carbonates from bio-sources such as epoxidized vegetable oils (EVOs) have significant challenges due to the low reactivity of CO2 and the steric hindrance of internal epoxides in these bulky substrates. Consequently, the majority of systems for CO2 fixation to bio-based epoxides rely on homogeneous catalysis. This study investigated the conversion of epoxidized methyl oleate, a model compound for EVOs, into its corresponding cyclic carbonate using heterogeneous 4-pyrrolidinopyridine-based catalysts. The influence of various catalytic parameters, such as the halide counter anions (Cl, Br, I) and incorporated metal Lewis acid centra, was explored within the catalyst. Among the halide counter anions, bromide exhibited a superior performance, achieving 65 % conversion and 59 % cyclic carbonate yield by the end of the experiment, while the effect of various metal centra was less pronounced, with an overall improvement in the cyclic carbonate yield of less than 10 % compared to the metal-free catalyst. A comprehensive study of reaction parameters, including the temperature (100–170°C), the CO2 pressure (20–40 bar), and the catalyst loading (2.9–10.7 wt%), was conducted in a laboratory-scale autoclave reactor to elucidate the behavior of the reaction system.
{"title":"A pathway to cyclic carbonates: Cycloaddition of carbon dioxide to epoxidized methyl oleate on grafted heterogeneous catalysts","authors":"Wander Y. Perez-Sena , Fabrizio Ciccarelli , Kari Eränen , Martino Di Serio , Vincenzo Russo , Tapio Salmi","doi":"10.1016/j.jcou.2024.103005","DOIUrl":"10.1016/j.jcou.2024.103005","url":null,"abstract":"<div><div>The conversion of CO<sub>2</sub> into value-added cyclic carbonates via cycloaddition to bio-derived epoxides presents a sustainable approach for CO<sub>2</sub> utilization. However, the production of cyclic carbonates from bio-sources such as epoxidized vegetable oils (EVOs) have significant challenges due to the low reactivity of CO<sub>2</sub> and the steric hindrance of internal epoxides in these bulky substrates. Consequently, the majority of systems for CO<sub>2</sub> fixation to bio-based epoxides rely on homogeneous catalysis. This study investigated the conversion of epoxidized methyl oleate, a model compound for EVOs, into its corresponding cyclic carbonate using heterogeneous 4-pyrrolidinopyridine-based catalysts. The influence of various catalytic parameters, such as the halide counter anions (Cl, Br, I) and incorporated metal Lewis acid centra, was explored within the catalyst. Among the halide counter anions, bromide exhibited a superior performance, achieving 65 % conversion and 59 % cyclic carbonate yield by the end of the experiment, while the effect of various metal centra was less pronounced, with an overall improvement in the cyclic carbonate yield of less than 10 % compared to the metal-free catalyst. A comprehensive study of reaction parameters, including the temperature (100–170°C), the CO<sub>2</sub> pressure (20–40 bar), and the catalyst loading (2.9–10.7 wt%), was conducted in a laboratory-scale autoclave reactor to elucidate the behavior of the reaction system.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"91 ","pages":"Article 103005"},"PeriodicalIF":7.2,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143177108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.jcou.2024.103002
Tianhui Fan , Siyu Shen , Chun Yat (Benjamin) Sit , Paul J.A. Kenis , Andrew Chapman
Technological solutions to address climate change are coalescing around renewable energy deployment. Yet, the deployment of renewables alone may not be sufficient to restrict temperature increases in line with Paris Agreement targets. The emergence of carbon negative technologies to bridge this shortfall is needed and expected to overcome this gap. Among these technologies, direct air capture (DAC) is being deployed at multiple scales using various approaches. This study investigates membrane-based DAC integrated with subsequent carbon dioxide to carbon fuel conversion, i.e., DAC with utilization (DAC-U). The DAC-U evaluation is undertaken holistically, beginning with a cradle-to-grave life cycle assessment, followed by economic feasibility scenario analysis and social acceptability analysis to establish acceptable deployment pricing and necessary policy interventions. This study reveals that, although the DAC-U represents a carbon negative capable technology with positive lifestyle and environmental outcomes, high capital costs present a significant barrier to deployment. To overcome this barrier, a robust policy regime including subsidies or fuel credits may be necessary. Further technological innovation and efficiency gains will also close this gap, meaning that the membrane-based DAC-U concept may play a role in achieving carbon neutrality goals in the near future.
{"title":"Environmental, economic and social trade-offs of membrane-based direct air capture technologies integrated with CO2 conversion using life cycle assessment","authors":"Tianhui Fan , Siyu Shen , Chun Yat (Benjamin) Sit , Paul J.A. Kenis , Andrew Chapman","doi":"10.1016/j.jcou.2024.103002","DOIUrl":"10.1016/j.jcou.2024.103002","url":null,"abstract":"<div><div>Technological solutions to address climate change are coalescing around renewable energy deployment. Yet, the deployment of renewables alone may not be sufficient to restrict temperature increases in line with Paris Agreement targets. The emergence of carbon negative technologies to bridge this shortfall is needed and expected to overcome this gap. Among these technologies, direct air capture (DAC) is being deployed at multiple scales using various approaches. This study investigates membrane-based DAC integrated with subsequent carbon dioxide to carbon fuel conversion, <em>i.e.</em>, DAC with utilization (DAC-U). The DAC-U evaluation is undertaken holistically, beginning with a cradle-to-grave life cycle assessment, followed by economic feasibility scenario analysis and social acceptability analysis to establish acceptable deployment pricing and necessary policy interventions. This study reveals that, although the DAC-U represents a carbon negative capable technology with positive lifestyle and environmental outcomes, high capital costs present a significant barrier to deployment. To overcome this barrier, a robust policy regime including subsidies or fuel credits may be necessary. Further technological innovation and efficiency gains will also close this gap, meaning that the membrane-based DAC-U concept may play a role in achieving carbon neutrality goals in the near future.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"91 ","pages":"Article 103002"},"PeriodicalIF":7.2,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143177102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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