Pub Date : 2025-10-14DOI: 10.1016/j.jcou.2025.103234
R.B. Machado-Silva, C. Cerdá-Moreno, A. Chica
The influence of Ni incorporation methods and metal loading on sepiolite-based catalysts for the CO2 methanation reaction was investigated. Catalysts synthesized via precipitation exhibited a Ni phase strongly interacting with a partially folded sepiolite structure, as revealed by ²⁹Si-NMR and TPR analyses, distinct from those obtained by incipient wetness impregnation. The precipitation method resulted in catalysts with enhanced reducibility and a fourfold increase in Ni0 surface area, as confirmed by XPS and H2-chemisorption measurements, which correlated with higher CO2 conversion and CH4 selectivity observed. Among the precipitation-based catalysts, the one with 20 wt% Ni loading exhibited the optimal balance between Ni⁰ surface area (13.6 m² gCAT−1) and catalytic performance (0.233 mol CH4 gCAT−1 h−1, at 400 °C). Stability tests demonstrated that this catalyst maintained a steady CH4 yield over 24 h of continuous operation.
{"title":"Rational design of Ni-sepiolite catalysts: Impact of incorporation method and metal loading on CO2 methanation efficiency","authors":"R.B. Machado-Silva, C. Cerdá-Moreno, A. Chica","doi":"10.1016/j.jcou.2025.103234","DOIUrl":"10.1016/j.jcou.2025.103234","url":null,"abstract":"<div><div>The influence of Ni incorporation methods and metal loading on sepiolite-based catalysts for the CO<sub>2</sub> methanation reaction was investigated. Catalysts synthesized via precipitation exhibited a Ni phase strongly interacting with a partially folded sepiolite structure, as revealed by ²⁹Si-NMR and TPR analyses, distinct from those obtained by incipient wetness impregnation. The precipitation method resulted in catalysts with enhanced reducibility and a fourfold increase in Ni<sup>0</sup> surface area, as confirmed by XPS and H<sub>2</sub>-chemisorption measurements, which correlated with higher CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity observed. Among the precipitation-based catalysts, the one with 20 wt% Ni loading exhibited the optimal balance between Ni⁰ surface area (13.6 m² g<sub>CAT</sub><sup>−1</sup>) and catalytic performance (0.233 mol CH<sub>4</sub> g<sub>CAT</sub><sup>−1</sup> h<sup>−1</sup>, at 400 °C). Stability tests demonstrated that this catalyst maintained a steady CH<sub>4</sub> yield over 24 h of continuous operation.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103234"},"PeriodicalIF":8.4,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145321278","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 : 2025-10-13DOI: 10.1016/j.jcou.2025.103235
Azmat Ali Khan, Muhammad Tahir
A well-designed trimetallic CoAlLa layered double hydroxide (CoAlLa-LDH), having a high number of active sites and oxygen defects, with multilayered Ti₃C₂ MXene and TiO₂ nanoparticles, was synthesized through heterojunction engineering to enhance CO₂ photoreduction. The strong interaction between a p-type CoAlLa-LDH and an n-type TiO₂, resulting in the formation of a distinctive S-scheme heterojunction, effectively promotes charge separation by reducing electron-hole recombination due to the multilayered Ti3C2 MXenes. The photocatalytic conversion of CO₂ with H₂O resulted in the production of CO and CH₄ of 38.25 and 3.36 µmol in 4 h, respectively. The photocatalytic performance over optimized Ti₃C₂/CoAlLa-LDH/TiO₂ nanocomposite was 3.6 and 4.3 for CO and 2.64 and 3.28 for CH4, respectively, higher than TiO₂ and LDH materials. The performance improvement was attributed to the construction of a heterostructure that offered abundant active sites, and the strong connection between nanomaterials, endorsing the generation of an electric field and hastening the transport of generated charge carriers. Furthermore, stability tests confirmed high stability of the CoAlLa-LDH/Ti₃C₂/TiO₂ nanocomposite over multiple cycles, demonstrating its long-term activation as a photocatalyst. This work not only provides a new pathway for designing highly efficient photocatalysts but also offers insightful guidance for future advancements in sustainable energy conversion and carbon-neutral technologies.
{"title":"Engineered dual-interface MXene-integrated CoAlLa-LDH/TiO₂ ternary heterojunctions for highly selective photoreduction of CO₂ into renewable fuels","authors":"Azmat Ali Khan, Muhammad Tahir","doi":"10.1016/j.jcou.2025.103235","DOIUrl":"10.1016/j.jcou.2025.103235","url":null,"abstract":"<div><div>A well-designed trimetallic CoAlLa layered double hydroxide (CoAlLa-LDH), having a high number of active sites and oxygen defects, with multilayered Ti₃C₂ MXene and TiO₂ nanoparticles, was synthesized through heterojunction engineering to enhance CO₂ photoreduction. The strong interaction between a p-type CoAlLa-LDH and an n-type TiO₂, resulting in the formation of a distinctive S-scheme heterojunction, effectively promotes charge separation by reducing electron-hole recombination due to the multilayered Ti<sub>3</sub>C<sub>2</sub> MXenes. The photocatalytic conversion of CO₂ with H₂O resulted in the production of CO and CH₄ of 38.25 and 3.36 µmol in 4 h, respectively. The photocatalytic performance over optimized Ti₃C₂/CoAlLa-LDH/TiO₂ nanocomposite was 3.6 and 4.3 for CO and 2.64 and 3.28 for CH<sub>4,</sub> respectively, higher than TiO₂ and LDH materials. The performance improvement was attributed to the construction of a heterostructure that offered abundant active sites, and the strong connection between nanomaterials, endorsing the generation of an electric field and hastening the transport of generated charge carriers. Furthermore, stability tests confirmed high stability of the CoAlLa-LDH/Ti₃C₂/TiO₂ nanocomposite over multiple cycles, demonstrating its long-term activation as a photocatalyst. This work not only provides a new pathway for designing highly efficient photocatalysts but also offers insightful guidance for future advancements in sustainable energy conversion and carbon-neutral technologies.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103235"},"PeriodicalIF":8.4,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145321279","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 : 2025-10-13DOI: 10.1016/j.jcou.2025.103247
Chaudhri Abdur Raheem, Muhammad Huzaifa, Muhammad Qasim Shafique, Muhammad Fahim Khokhar
This study aimed to develop a low-cost, circular route for sustainable methanol production by coupling capture of CO₂ from waste polypropylene surgical masks with solar-driven conversion. Used masks were upcycled into activated carbon that adsorbed CO₂ at 2.711 mmol g⁻¹ . The captured CO₂ was reduced to methanol using a copper–carbon co-doped titanium dioxide (Cu–C/TiO₂) photocatalyst operated under ultraviolet (UV) light and natural sunlight in a compact integrated CO₂-to-methanol photoreactor. Relative to commercial TiO₂, the co-doped catalyst increased methanol productivity by about sixfold. After 5 h, methanol concentrations reached 3.79 g L⁻¹ under UV irradiation and 3.39 g L⁻¹ under sunlight. Using seawater as the reaction medium provided the highest yield, though it posed regeneration challenges, while the catalyst maintained 98.6 % of its activity after regeneration. A laboratory-scale carbon balance indicated near carbon-neutral performance for the conversion step, and analysis suggests a path to carbon-negative operation at scale by combining avoided mask incineration with sustained CO₂ capture. These results demonstrate that upcycling mask waste into an efficient CO₂ sorbent and pairing it with a regenerable photocatalyst can produce methanol under mild conditions using low-cost hardware, offering a practical carbon capture and utilization pathway that simultaneously mitigates plastic waste and greenhouse-gas emissions.
本研究旨在通过将废弃聚丙烯外科口罩中的二氧化碳捕获与太阳能驱动的转换相结合，开发一种低成本、循环的可持续甲醇生产路线。用过的口罩被升级为活性炭，吸附CO₂的浓度为2.711 mmol g⁻¹ 。采用铜碳共掺杂二氧化钛（Cu-C /TiO 2）光催化剂，在紫外（UV）光和自然光下，在紧凑的集成CO 2 -甲醇光反应器中将捕获的CO 2还原为甲醇。与商业二氧化钛相比，共掺杂催化剂使甲醇产率提高了约6倍。5 h后，紫外线照射下的甲醇浓度达到3.79 g L⁻¹ ，阳光照射下的甲醇浓度达到3.39 g L⁻¹ 。以海水为反应介质产率最高，但存在再生挑战，再生后催化剂的活性保持在98.6 %。实验室规模的碳平衡表明，转化步骤的性能接近碳中和，分析表明，通过将避免的面罩焚烧与持续的CO 2捕获相结合，可以实现大规模的碳负操作。这些结果表明，将面罩废物升级为高效的CO 2吸附剂，并将其与可再生光催化剂相结合，可以在温和的条件下使用低成本的硬件生产甲醇，提供了一种实用的碳捕获和利用途径，同时减少了塑料废物和温室气体排放。
{"title":"Sustainable methanol production from CO2 using waste mask-derived activated carbon and Cu–C/TiO2 photocatalyst","authors":"Chaudhri Abdur Raheem, Muhammad Huzaifa, Muhammad Qasim Shafique, Muhammad Fahim Khokhar","doi":"10.1016/j.jcou.2025.103247","DOIUrl":"10.1016/j.jcou.2025.103247","url":null,"abstract":"<div><div>This study aimed to develop a low-cost, circular route for sustainable methanol production by coupling capture of CO₂ from waste polypropylene surgical masks with solar-driven conversion. Used masks were upcycled into activated carbon that adsorbed CO₂ at 2.711 mmol g⁻¹ . The captured CO₂ was reduced to methanol using a copper–carbon co-doped titanium dioxide (Cu–C/TiO₂) photocatalyst operated under ultraviolet (UV) light and natural sunlight in a compact integrated CO₂-to-methanol photoreactor. Relative to commercial TiO₂, the co-doped catalyst increased methanol productivity by about sixfold. After 5 h, methanol concentrations reached 3.79 g L⁻¹ under UV irradiation and 3.39 g L⁻¹ under sunlight. Using seawater as the reaction medium provided the highest yield, though it posed regeneration challenges, while the catalyst maintained 98.6 % of its activity after regeneration. A laboratory-scale carbon balance indicated near carbon-neutral performance for the conversion step, and analysis suggests a path to carbon-negative operation at scale by combining avoided mask incineration with sustained CO₂ capture. These results demonstrate that upcycling mask waste into an efficient CO₂ sorbent and pairing it with a regenerable photocatalyst can produce methanol under mild conditions using low-cost hardware, offering a practical carbon capture and utilization pathway that simultaneously mitigates plastic waste and greenhouse-gas emissions.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103247"},"PeriodicalIF":8.4,"publicationDate":"2025-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145321373","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 : 2025-10-11DOI: 10.1016/j.jcou.2025.103245
Seyed Ghasem Rezvannasab , Navid Safari , Abdol Mohammad Ghaedi
In this study, a composite of Graphene Oxide, Magnesium Oxide, and Polyethyleneimine (GO/MgO/PEI) was synthesized and utilized as a novel adsorbent for CO2 capture. Material characterization was performed using XRD, FTIR, FE-SEM, TGA, and BET analysis. The composite achieved a maximum CO2 adsorption capacity of 291.70 mg/g at 298 K and 8.7 bar, with an optimal GO-MgO ratio of 1:1 and PEI at 3 wt%. Operating parameters such as temperature, pressure, and PEI concentration were examined and optimized using response surface methodology with a Box–Behnken design (RSM-BBD). Analysis of variance indicated that all input variables significantly affected the CO2 uptake process. The strong correlation between the CO2 uptake process and the model was demonstrated by an R² value of 0.9946. Isotherm and kinetic studies revealed that the Sips and Pseudo second-order models best represented the CO2 adsorption behavior. Furthermore, thermodynamic analysis indicated that the process was exothermic, spontaneous, and physical in nature. Additionally, recyclability tests showed only a small reduction in CO2 adsorption efficiency after 20 cycles, suggesting promising performance for industrial applications.
{"title":"Synthesis and performance enhancement of GO/MgO/PEI composite for CO₂ capture: Effects of operating parameters","authors":"Seyed Ghasem Rezvannasab , Navid Safari , Abdol Mohammad Ghaedi","doi":"10.1016/j.jcou.2025.103245","DOIUrl":"10.1016/j.jcou.2025.103245","url":null,"abstract":"<div><div>In this study, a composite of Graphene Oxide, Magnesium Oxide, and Polyethyleneimine (GO/MgO/PEI) was synthesized and utilized as a novel adsorbent for CO2 capture. Material characterization was performed using XRD, FTIR, FE-SEM, TGA, and BET analysis. The composite achieved a maximum CO2 adsorption capacity of 291.70 mg/g at 298 K and 8.7 bar, with an optimal GO-MgO ratio of 1:1 and PEI at 3 wt%. Operating parameters such as temperature, pressure, and PEI concentration were examined and optimized using response surface methodology with a Box–Behnken design (RSM-BBD). Analysis of variance indicated that all input variables significantly affected the CO2 uptake process. The strong correlation between the CO2 uptake process and the model was demonstrated by an R² value of 0.9946. Isotherm and kinetic studies revealed that the Sips and Pseudo second-order models best represented the CO2 adsorption behavior. Furthermore, thermodynamic analysis indicated that the process was exothermic, spontaneous, and physical in nature. Additionally, recyclability tests showed only a small reduction in CO2 adsorption efficiency after 20 cycles, suggesting promising performance for industrial applications.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103245"},"PeriodicalIF":8.4,"publicationDate":"2025-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263358","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 : 2025-10-10DOI: 10.1016/j.jcou.2025.103239
Yong Liu , Junhui Bai , Yubo Lan , Jiang Zhang , Sen Liu , Jian Wang , Fajun Zhao
CO₂ foam flooding is a promising enhanced oil recovery (EOR) technique for improving sweep efficiency and mitigating gas channeling in heterogeneous reservoirs and the solubility behavior of surfactants plays a critical role in determining foam formation and stability. In this study, a representative CO₂-soluble surfactant was investigated under high-pressure conditions. Solubility tests, foam performance evaluation, and interfacial tension measurements were conducted to systematically examine the effects of surfactant solubility and dissolution rate on foam volume and stability. The results showed that at 60 °C and 22 MPa, the surfactant exhibited a CO₂-phase solubility of up to 2.4 %, which decreased to approximately 1.1 % at 90 °C under the same pressure. As the pressure increased from 8 MPa to 22 MPa, the foam half-life extended from 70 min to nearly 500 min, and the foam comprehensive index increased from 1000 mL·min to over 4000 mL·min, indicating significant performance enhancement. Additionally, as the surfactant concentration increased from 0 % to 1.2 %, interfacial tension decreased substantially, and the minimum miscibility pressure (MMP) dropped from 31.4 MPa to 27.6 MPa. Further analysis revealed that the surfactant improves foam film formation and stability through a synergistic mechanism involving “dissolution–transport–precipitation–interfacial activity regulation.” These findings provide both theoretical insights and practical guidance for the design and screening of efficient surfactants in CO₂ foam flooding applications.
{"title":"Synergistic mechanism of CO₂-soluble surfactant dissolution and foam formation under high-pressure conditions","authors":"Yong Liu , Junhui Bai , Yubo Lan , Jiang Zhang , Sen Liu , Jian Wang , Fajun Zhao","doi":"10.1016/j.jcou.2025.103239","DOIUrl":"10.1016/j.jcou.2025.103239","url":null,"abstract":"<div><div>CO₂ foam flooding is a promising enhanced oil recovery (EOR) technique for improving sweep efficiency and mitigating gas channeling in heterogeneous reservoirs and the solubility behavior of surfactants plays a critical role in determining foam formation and stability. In this study, a representative CO₂-soluble surfactant was investigated under high-pressure conditions. Solubility tests, foam performance evaluation, and interfacial tension measurements were conducted to systematically examine the effects of surfactant solubility and dissolution rate on foam volume and stability. The results showed that at 60 °C and 22 MPa, the surfactant exhibited a CO₂-phase solubility of up to 2.4 %, which decreased to approximately 1.1 % at 90 °C under the same pressure. As the pressure increased from 8 MPa to 22 MPa, the foam half-life extended from 70 min to nearly 500 min, and the foam comprehensive index increased from 1000 mL·min to over 4000 mL·min, indicating significant performance enhancement. Additionally, as the surfactant concentration increased from 0 % to 1.2 %, interfacial tension decreased substantially, and the minimum miscibility pressure (MMP) dropped from 31.4 MPa to 27.6 MPa. Further analysis revealed that the surfactant improves foam film formation and stability through a synergistic mechanism involving “dissolution–transport–precipitation–interfacial activity regulation.” These findings provide both theoretical insights and practical guidance for the design and screening of efficient surfactants in CO₂ foam flooding applications.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103239"},"PeriodicalIF":8.4,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263359","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}
Thermodynamic equilibrium analysis is a powerful tool for assessing the feasibility of chemical reactions and product distributions under different operating conditions. This study investigates the feasibility and intrinsic nature of each possible reaction in CO2 hydrogenation using the equilibrium constant (K) method and calculating thermodynamic parameters. In addition, the equilibrium product distribution and CO2 conversion of CO2 hydrogenation to light olefins (CTO) process determined at temperature range of 200–400℃, pressure of 1–50 bar, and different H2/CO2 feed ratios (1, 2, 3, and 4) using Gibbs free energy (GFE) minimization method. The results indicate that, elevated temperatures strongly promote the formation of light olefins while effectively suppressing coke deposition, pressure exerts a moderate enhancing effect, and a higher H2/CO2 ratio, particularly at lower temperatures, significantly reduces coke formation while having only a minor influence on light olefins selectivity. In contrast, CO2 conversion decreases markedly with increasing temperature, while higher pressure and elevated H2/CO2 ratios enhance the conversion. Ultimately, the maximum selectivity of light olefins (1.22 ×10−7) was obtained at 400℃, 50 bar, and H2/CO2 = 3, under which coke formation was completely suppressed, although the corresponding CO2 conversion was only 7.6 %. These findings highlight not only the intrinsic nature of the CTO process and the influence of operating conditions on its equilibrium product distribution, but also provide valuable guidance for catalyst development in the absence of extensive experiments.
{"title":"A comprehensive thermodynamic equilibrium analysis of direct CO2 hydrogenation to light olefins product","authors":"Farshid Sobhani Bazghaleh, Jafar Towfighi Darian, Yosef Niktab, Masoud Safari Yazd","doi":"10.1016/j.jcou.2025.103238","DOIUrl":"10.1016/j.jcou.2025.103238","url":null,"abstract":"<div><div>Thermodynamic equilibrium analysis is a powerful tool for assessing the feasibility of chemical reactions and product distributions under different operating conditions. This study investigates the feasibility and intrinsic nature of each possible reaction in CO<sub>2</sub> hydrogenation using the equilibrium constant (K) method and calculating thermodynamic parameters. In addition, the equilibrium product distribution and CO<sub>2</sub> conversion of CO<sub>2</sub> hydrogenation to light olefins (CTO) process determined at temperature range of 200–400℃, pressure of 1–50 bar, and different H<sub>2</sub>/CO<sub>2</sub> feed ratios (1, 2, 3, and 4) using Gibbs free energy (GFE) minimization method. The results indicate that, elevated temperatures strongly promote the formation of light olefins while effectively suppressing coke deposition, pressure exerts a moderate enhancing effect, and a higher H<sub>2</sub>/CO<sub>2</sub> ratio, particularly at lower temperatures, significantly reduces coke formation while having only a minor influence on light olefins selectivity. In contrast, CO<sub>2</sub> conversion decreases markedly with increasing temperature, while higher pressure and elevated H<sub>2</sub>/CO<sub>2</sub> ratios enhance the conversion. Ultimately, the maximum selectivity of light olefins (1.22 ×10<sup>−7</sup>) was obtained at 400℃, 50 bar, and H<sub>2</sub>/CO<sub>2</sub> = 3, under which coke formation was completely suppressed, although the corresponding CO<sub>2</sub> conversion was only 7.6 %. These findings highlight not only the intrinsic nature of the CTO process and the influence of operating conditions on its equilibrium product distribution, but also provide valuable guidance for catalyst development in the absence of extensive experiments.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103238"},"PeriodicalIF":8.4,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263357","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 : 2025-10-09DOI: 10.1016/j.jcou.2025.103241
Kihyuk Sung , Hye Jeong Joe , Changsu Ha , Hee-Seong Yang , In-Hwan Lee , Seok Ki Kim , Hye-Young Jang
We investigated the polymerization mechanism of a highly active heterogeneous Zn-gallate catalyst used for propylene oxide (PO) homopolymerization and PO/CO2 copolymerization. The molecular weights of poly(propylene oxide) (PPO) and poly(propylene carbonate) (PPC) can be controlled by varying the ratio of chain transfer agents (CTAs) to PO. CTAs of varying acidity and structure provided insight into their interaction with catalytic sites. Theoretical calculations on a heterogeneous zinc hydroxide slab model for Zn-gallate revealed that polymerization is initiated by the reaction of PO with a hydroxyl group located within the zinc hydroxide lattice. Further energy barrier calculations and polymerizations at varying CO2 pressures explained the kinetic preference for PPC formation over PPO at high CO2 pressure.
{"title":"Understanding heterogeneous Zn-gallate catalyzed copolymerization of propylene oxide and CO2","authors":"Kihyuk Sung , Hye Jeong Joe , Changsu Ha , Hee-Seong Yang , In-Hwan Lee , Seok Ki Kim , Hye-Young Jang","doi":"10.1016/j.jcou.2025.103241","DOIUrl":"10.1016/j.jcou.2025.103241","url":null,"abstract":"<div><div>We investigated the polymerization mechanism of a highly active heterogeneous Zn-gallate catalyst used for propylene oxide (PO) homopolymerization and PO/CO<sub>2</sub> copolymerization. The molecular weights of poly(propylene oxide) (PPO) and poly(propylene carbonate) (PPC) can be controlled by varying the ratio of chain transfer agents (CTAs) to PO. CTAs of varying acidity and structure provided insight into their interaction with catalytic sites. Theoretical calculations on a heterogeneous zinc hydroxide slab model for Zn-gallate revealed that polymerization is initiated by the reaction of PO with a hydroxyl group located within the zinc hydroxide lattice. Further energy barrier calculations and polymerizations at varying CO<sub>2</sub> pressures explained the kinetic preference for PPC formation over PPO at high CO<sub>2</sub> pressure.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103241"},"PeriodicalIF":8.4,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263360","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}
Supercritical fluid impregnation (SFI) is well-documented at lab-scale; however, applications at pilot-scale remain scarce. This study aims to address the gap by investigating the pilot-scale impregnation of biodegradable polylactic acid/poly(butylene adipate-co-terephthalate)/thermoplastic starch (PLA/PBAT/TPS) films using olive leaf extract. The extract of Olea europaea L. leaves was obtained using enhanced solvent extraction. It is a source of pigments and polyphenols, with a concentration of 115 ± 2 mg ml−1 and an EC50 of 33 ± 3 μg ml−1. The SFI of PLA/PBAT/TPS films was optimized at lab scale, being 250 bar and 35 °C, the optimal conditions. Under these conditions, SFI was scaled 4-fold, and the effects of extract volume, film surface area, and contact time were evaluated. The quality of the films was assessed based on impregnation homogeneity, extract loading, chemical composition and antioxidant activity against 2,2 ´ -azinobis(3-ethylbenzothiazoline-6-sulfonic) (ABTS). The films impregnated at pilot scale showed optimal results using 30 ml of extract, a 1360 cm2 film, and 1 h of contact time, achieving an extract loading (1.41 ± 0.08 mg cm−2) and antioxidant activity (52 ± 4 %) comparable to those at lab scale. The results confirmed the successful impregnation of polyphenols and suggested interactions between extract compounds and polymer carbonyl groups. Chlorophylls aided the assessment of impregnation homogeneity, a critical factor for product quality, which proved to be consistent throughout the film as the scale was increased. These findings confirm the technical feasibility of SFI at pilot scale and support its potential for sustainable production of bioactive packaging materials.
{"title":"Pilot-scale supercritical CO₂ impregnation for functionalization of biodegradable PLA/PBAT/TPS films","authors":"Noelia D. Machado, Inmaculada Domínguez-Gómez, Cristina Cejudo-Bastante, Casimiro Mantell-Serrano, Lourdes Casas-Cardoso","doi":"10.1016/j.jcou.2025.103242","DOIUrl":"10.1016/j.jcou.2025.103242","url":null,"abstract":"<div><div>Supercritical fluid impregnation (SFI) is well-documented at lab-scale; however, applications at pilot-scale remain scarce. This study aims to address the gap by investigating the pilot-scale impregnation of biodegradable polylactic acid/poly(butylene adipate-co-terephthalate)/thermoplastic starch (PLA/PBAT/TPS) films using olive leaf extract. The extract of <em>Olea europaea</em> L. leaves was obtained using enhanced solvent extraction. It is a source of pigments and polyphenols, with a concentration of 115 ± 2 mg ml<sup>−1</sup> and an EC<sub>50</sub> of 33 ± 3 μg ml<sup>−1</sup>. The SFI of PLA/PBAT/TPS films was optimized at lab scale, being 250 bar and 35 °C, the optimal conditions. Under these conditions, SFI was scaled 4-fold, and the effects of extract volume, film surface area, and contact time were evaluated. The quality of the films was assessed based on impregnation homogeneity, extract loading, chemical composition and antioxidant activity against 2,2 ´ -azinobis(3-ethylbenzothiazoline-6-sulfonic) (ABTS). The films impregnated at pilot scale showed optimal results using 30 ml of extract, a 1360 cm<sup>2</sup> film, and 1 h of contact time, achieving an extract loading (1.41 ± 0.08 mg cm<sup>−2</sup>) and antioxidant activity (52 ± 4 %) comparable to those at lab scale. The results confirmed the successful impregnation of polyphenols and suggested interactions between extract compounds and polymer carbonyl groups. Chlorophylls aided the assessment of impregnation homogeneity, a critical factor for product quality, which proved to be consistent throughout the film as the scale was increased. These findings confirm the technical feasibility of SFI at pilot scale and support its potential for sustainable production of bioactive packaging materials.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103242"},"PeriodicalIF":8.4,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263361","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 : 2025-10-06DOI: 10.1016/j.jcou.2025.103233
Ning Kang , Bauyrzhan Sarsenbekuly , Hairong Wu
Carbon Capture, Utilization, and Storage (CCUS) technology has emerged as a pivotal approach for reducing carbon emissions. In recent years, the application of CCUS in oilfield operations has gained significant momentum. This paper provides a comprehensive review of recent advancements in CO₂ capture technologies, analyzing their respective advantages and disadvantages. It also examines the challenges associated with CO₂ transportation technologies, with a particular focus on CO₂ flooding for enhanced oil recovery (EOR). The mechanisms of CO₂ flooding, including miscible, near-miscible, and immiscible displacement, are discussed in detail, along with the application status of various CO₂ sealing and carbon storage technologies in domestic and international oilfields. Finally, the challenges hindering the large-scale industrial application of CCUS in oilfields are summarized, and its potential for improving oil recovery and carbon storage processes is explored. This study holds significant implications for advancing CO₂ flooding and storage technologies, enhancing the utilization and recovery rates of low-permeability reservoirs, ensuring national energy security, and mitigating carbon emissions.
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Pub Date : 2025-10-06DOI: 10.1016/j.jcou.2025.103237
Ruwei Yao, Bin Wu, Yueyin Song, Qinqin Niu, Zhuoyi Yang, Han Zhang, Congming Li
Directly converting CO2 into higher alcohols through catalytic hydrogenation offers a sustainable pathway for carbon recycling and renewable energy storage. CuFe-based catalysts have shown particular promise for this process, with the performance being predominantly governed by interfacial synergy between metal sites. In this study, the role of Zn as a spatial and electronic modifier in CuFe catalysts is investigated by systematically exploring a broad range of Zn incorporation levels. The optimized Zn(3)-CuFeK catalyst exhibits superior performance with 20 % alcohol selectivity and a space-time yield of 121.2 mg gcat-1 h-1, representing a nearly 50 % enhancement over the Zn-free counterpart. Detailed characterizations reveal that moderate Zn incorporation can improve metal dispersion and promote catalytic synergy at Cu-Fe interfacial sites, while Zn-induced electronic modulation increases electron density around Cu sites and stabilizes the adsorbed non-dissociated *CO species. The spatial and electronic effects synergistically promote the challenging C−C coupling between *CO and alkyl species, thereby boosting alcohol production. Temperature-programmed surface reaction (TPSR) and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy provide direct evidence for the role of Zn in enhancing both the relative concentration and stability of the crucial non-dissociated *CO species.
{"title":"Unraveling the role of zinc in CuFe-based catalysts for CO2 hydrogenation to higher alcohols","authors":"Ruwei Yao, Bin Wu, Yueyin Song, Qinqin Niu, Zhuoyi Yang, Han Zhang, Congming Li","doi":"10.1016/j.jcou.2025.103237","DOIUrl":"10.1016/j.jcou.2025.103237","url":null,"abstract":"<div><div>Directly converting CO<sub>2</sub> into higher alcohols through catalytic hydrogenation offers a sustainable pathway for carbon recycling and renewable energy storage. CuFe-based catalysts have shown particular promise for this process, with the performance being predominantly governed by interfacial synergy between metal sites. In this study, the role of Zn as a spatial and electronic modifier in CuFe catalysts is investigated by systematically exploring a broad range of Zn incorporation levels. The optimized Zn(3)-CuFeK catalyst exhibits superior performance with 20 % alcohol selectivity and a space-time yield of 121.2 mg g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, representing a nearly 50 % enhancement over the Zn-free counterpart. Detailed characterizations reveal that moderate Zn incorporation can improve metal dispersion and promote catalytic synergy at Cu-Fe interfacial sites, while Zn-induced electronic modulation increases electron density around Cu sites and stabilizes the adsorbed non-dissociated *CO species. The spatial and electronic effects synergistically promote the challenging C−C coupling between *CO and alkyl species, thereby boosting alcohol production. Temperature-programmed surface reaction (TPSR) and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy provide direct evidence for the role of Zn in enhancing both the relative concentration and stability of the crucial non-dissociated *CO species.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103237"},"PeriodicalIF":8.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263356","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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