Journal of CO2 Utilization最新文献_第7页

Pilot-scale supercritical CO₂ impregnation for functionalization of biodegradable PLA/PBAT/TPS films 超临界CO 2浸渍法制备可生物降解的PLA/PBAT/TPS膜

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-10-08 DOI: 10.1016/j.jcou.2025.103242

Noelia D. Machado, Inmaculada Domínguez-Gómez, Cristina Cejudo-Bastante, Casimiro Mantell-Serrano, Lourdes Casas-Cardoso

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.

超临界流体浸渍（SFI）在实验室规模上有很好的记录；然而，在中试规模上的应用仍然很少。本研究旨在通过研究橄榄叶提取物浸渍可生物降解聚乳酸/聚己二酸丁二酯/对苯二甲酸乙酯/热塑性淀粉（PLA/PBAT/TPS）薄膜的中试规模来解决这一空白。采用强化溶剂萃取法提取油橄榄叶提取物。它是色素和多酚的来源，浓度为115 ± 2 mg ml−1，EC50为33 ± 3 μg ml−1。在实验室条件下对PLA/PBAT/TPS薄膜的SFI进行了优化，最佳条件为250 bar和35℃。在此条件下，将SFI缩放4倍，并评估萃取量、膜表面积和接触时间对SFI的影响。通过浸渍均匀性、浸渍量、化学成分和抗2,2 ´ -氮唑啉（3-乙基苯并噻唑啉-6-磺酸）（ABTS）的抗氧化活性来评价膜的质量。中试浸渍膜的最佳浸渍时间为30 ml， 1360 cm2，接触时间为1 h，浸渍膜的浸渍量为1.41±0.08 mg cm−2，抗氧化活性为52±4 %，与实验室浸渍膜相当。结果证实了多酚的成功浸渍，并表明萃取物与聚合物羰基之间存在相互作用。叶绿素有助于评估浸渍均匀性，这是产品质量的关键因素，随着规模的增加，整个膜的浸渍均匀性证明是一致的。这些发现证实了SFI在中试规模上的技术可行性，并支持其可持续生产生物活性包装材料的潜力。

{"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}

引用次数: 0

Progress of CCUS technology with enhanced oil recovery 提高采收率的CCUS技术进展

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-10-06 DOI: 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.

碳捕获、利用和封存（CCUS）技术已成为减少碳排放的关键方法。近年来，CCUS在油田作业中的应用势头明显。本文全面综述了二氧化碳捕集技术的最新进展，分析了它们各自的优缺点。它还研究了与二氧化碳输送技术相关的挑战，特别关注二氧化碳驱油提高石油采收率（EOR）。详细论述了CO 2驱油机理，包括混相驱油、近混相驱油和非混相驱油，以及国内外油田各种CO 2封储技术的应用现状。最后，总结了阻碍CCUS在油田大规模工业应用的挑战，并探讨了CCUS在提高石油采收率和碳储存过程中的潜力。该研究对推进CO 2驱储技术、提高低渗透油藏的利用率和采收率、保障国家能源安全、减少碳排放具有重要意义。

{"title":"Progress of CCUS technology with enhanced oil recovery","authors":"Ning Kang , Bauyrzhan Sarsenbekuly , Hairong Wu","doi":"10.1016/j.jcou.2025.103233","DOIUrl":"10.1016/j.jcou.2025.103233","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103233"},"PeriodicalIF":8.4,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263362","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}

引用次数: 0

Unraveling the role of zinc in CuFe-based catalysts for CO2 hydrogenation to higher alcohols 揭示了锌在cufe基催化剂中二氧化碳加氢生成高级醇的作用

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-10-06 DOI: 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 g_cat^-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.

通过催化加氢直接将二氧化碳转化为高级醇，为碳回收和可再生能源储存提供了一条可持续的途径。基于cufe的催化剂在这一过程中表现出特别的前景，其性能主要由金属位点之间的界面协同作用决定。在本研究中，通过系统地探索广泛的锌掺入水平，研究了锌作为空间和电子改性剂在CuFe催化剂中的作用。优化后的Zn(3)-CuFeK催化剂表现出优异的性能，醇选择性为20% %，空时产率为121.2 mg gcat-1 h-1，比无Zn催化剂提高了近50% %。详细的表征表明，适量的Zn掺入可以改善Cu- fe界面位置的金属分散和促进催化协同作用，而Zn诱导的电子调制增加了Cu位置周围的电子密度，并稳定了吸附的未解离*CO。空间和电子效应协同促进了*CO和烷基之间具有挑战性的C - C耦合，从而促进了酒精的生产。温控表面反应（TPSR）和漫反射红外傅立叶变换（DRIFT）光谱为Zn在提高关键非解离*CO的相对浓度和稳定性方面的作用提供了直接证据。

{"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}

引用次数: 0

Bioadhesive design of CO2-based polycarbonate materials with thermosensitivity and biodegradability 具有热敏性和可生物降解性的co2基聚碳酸酯材料的生物粘合剂设计

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-30 DOI: 10.1016/j.jcou.2025.103236

Dake Zhang , Wenzhen Wang , Zhen Wang , Dengmeng Song , Shuang Liu , Yuyang Chen , Xiaoni Ma , Li Xia

Addressing the challenges of biotoxicity, poor long-term stability, and inadequate interfacial adhesion that hinder the clinical translation of tissue adhesives, we utilized the biocompatibility and biodegradability of CO₂-derived polycarbonates (PPC) and innovatively incorporated diacetyl-L-tartaric anhydride (DATA) into the copolymerization to develop PPC and DATA alternating/random copolymer (PPCD) bioadhesives. Compared to unmodified PPC, PPCD exhibits significantly enhanced adhesive properties: peel strength increased to 4.7 ± 0.43 N/cm (a 273 % improvement), sealing strength reached 67 ± 2.3 kPa (a 235 % enhancement), and skin adhesion strength rose to 22.1 ± 2.3 kPa (a 203 % increase). In comparative tests, PPCD outperformed commercial Fibrin glue in overall mechanical performance. Furthermore, PPCD demonstrates thermoresponsive viscosity modulation, undergoing debonding at 10°C with a thermal response efficiency exceeding 95 % compared to its viscosity at 37°C. Crucially, PPCD retains the degradability and bioaffinity of the original PPC, as confirmed by cytotoxicity assays showing > 98 % cell viability and histopathological analyses in mice verifying its biosafety. This bioadhesive resolves the long-standing trade-off between mechanical robustness and biocompatibility, while also establishing a new CO₂ valorization strategy for eco-friendly biomedical materials. The functionalization of PPC not only enhances adhesive performance but also pioneers a sustainable pathway for carbon utilization, demonstrating the transformative potential of next-generation tissue repair technologies.

针对生物毒性、长期稳定性差、界面粘附不足等阻碍组织粘接剂临床转化的挑战，我们利用CO₂衍生聚碳酸酯（PPC）的生物相容性和生物可降解性，创新地将二乙酰- l-酒石酸酐（DATA）加入共聚物中，开发了PPC和DATA交替/随机共聚物（PPCD）生物粘接剂。修改的PPC相比,PPCD展品显著增强胶粘剂性质:剥离强度增加到4.7 ±0.43  N /厘米(273 %改进),密封强度达到67 ± 2.3 kPa(235 %增强),和皮肤粘附强度升至22.1 ±2.3 kPa (增加203 %)。在对比试验中，PPCD在整体机械性能上优于市售纤维蛋白胶。此外，PPCD表现出热响应性粘度调制，在10°C时发生脱粘，与37°C时的粘度相比，热响应效率超过95% %。至关重要的是，PPCD保留了原始PPC的可降解性和生物亲和性，细胞毒性试验证实了>； 98 %的细胞存活率，小鼠组织病理学分析证实了其生物安全性。这种生物粘合剂解决了长期存在的机械坚固性和生物相容性之间的权衡，同时也为生态友好型生物医学材料建立了新的二氧化碳定价策略。PPC的功能化不仅提高了粘合性能，而且开创了碳利用的可持续途径，展示了下一代组织修复技术的变革潜力。

{"title":"Bioadhesive design of CO2-based polycarbonate materials with thermosensitivity and biodegradability","authors":"Dake Zhang , Wenzhen Wang , Zhen Wang , Dengmeng Song , Shuang Liu , Yuyang Chen , Xiaoni Ma , Li Xia","doi":"10.1016/j.jcou.2025.103236","DOIUrl":"10.1016/j.jcou.2025.103236","url":null,"abstract":"<div><div>Addressing the challenges of biotoxicity, poor long-term stability, and inadequate interfacial adhesion that hinder the clinical translation of tissue adhesives, we utilized the biocompatibility and biodegradability of CO₂-derived polycarbonates (PPC) and innovatively incorporated diacetyl-L-tartaric anhydride (DATA) into the copolymerization to develop PPC and DATA alternating/random copolymer (PPCD) bioadhesives. Compared to unmodified PPC, PPCD exhibits significantly enhanced adhesive properties: peel strength increased to 4.7 ± 0.43 N/cm (a 273 % improvement), sealing strength reached 67 ± 2.3 kPa (a 235 % enhancement), and skin adhesion strength rose to 22.1 ± 2.3 kPa (a 203 % increase). In comparative tests, PPCD outperformed commercial Fibrin glue in overall mechanical performance. Furthermore, PPCD demonstrates thermoresponsive viscosity modulation, undergoing debonding at 10°C with a thermal response efficiency exceeding 95 % compared to its viscosity at 37°C. Crucially, PPCD retains the degradability and bioaffinity of the original PPC, as confirmed by cytotoxicity assays showing > 98 % cell viability and histopathological analyses in mice verifying its biosafety. This bioadhesive resolves the long-standing trade-off between mechanical robustness and biocompatibility, while also establishing a new CO₂ valorization strategy for eco-friendly biomedical materials. The functionalization of PPC not only enhances adhesive performance but also pioneers a sustainable pathway for carbon utilization, demonstrating the transformative potential of next-generation tissue repair technologies.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103236"},"PeriodicalIF":8.4,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217711","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}

引用次数: 0

Optimizing hydrogen production from wastewater-derived sewage sludge via alkali-catalyzed supercritical water gasification 碱催化超临界水气化废水污泥制氢优化研究

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-29 DOI: 10.1016/j.jcou.2025.103232

S. Dhivya , Mohamed Ben Ammar , Murad Irshied Al-Maaitah , Rebwar Nasir Dara , A. Anderson , Likius Shipwiisho Daniel , Thandiwe Sithole , Kassian T.T. Amesho

The increasing global wastewater generation and reliance on fossil fuels for energy production necessitate sustainable treatment and energy recovery solutions. This study explores supercritical water gasification (SCWG) of sewage sludge from municipal wastewater as a hydrogen production pathway, focusing on the role of alkali catalysts (KOH, K₂CO₃, Na₂CO₃). The effects of temperature (450–550°C), reaction time (5–30 min), and catalyst type on gas yield and efficiency were analyzed. At 550°C, the highest carbon efficiency (61 %), gas efficiency (69 %), and hydrogen yield (41 mol/kg) were observed. After 30 min, the gas composition reached H₂ (58 %), CO₂ (26 %), CH₄ (11.7 %), and CO (4 %). Among catalysts, Na₂CO₃ exhibited superior H₂ yield (29 mol/kg), carbon efficiency (58 %), and gas efficiency (51 %). This study highlights SCWG as a viable technology for hydrogen-rich gas production, contributing to sustainable energy solutions and wastewater valorization.

随着全球废水产生量的增加和能源生产对化石燃料的依赖，需要可持续的处理和能源回收解决方案。本研究探讨了城市污水污泥的超临界水气化（SCWG）作为制氢途径，重点研究了碱催化剂（KOH, K₂CO₃，Na₂CO₃）的作用。分析了温度（450 ~ 550℃）、反应时间（5 ~ 30 min）和催化剂类型对产气率和效率的影响。在550°C时，观察到最高的碳效率（61 %）、气效率（69 %）和产氢率（41 mol/kg）。30 min后，气体组成为H₂（58 %）、CO₂（26 %）、CH₄（11.7 %）和CO（4 %）。在催化剂中，Na₂CO₃具有较好的H₂产率（29 mol/kg）、碳效率（58 %）和气体效率（51 %）。该研究强调了SCWG作为一种可行的富氢气生产技术，有助于可持续能源解决方案和废水增值。

{"title":"Optimizing hydrogen production from wastewater-derived sewage sludge via alkali-catalyzed supercritical water gasification","authors":"S. Dhivya , Mohamed Ben Ammar , Murad Irshied Al-Maaitah , Rebwar Nasir Dara , A. Anderson , Likius Shipwiisho Daniel , Thandiwe Sithole , Kassian T.T. Amesho","doi":"10.1016/j.jcou.2025.103232","DOIUrl":"10.1016/j.jcou.2025.103232","url":null,"abstract":"<div><div>The increasing global wastewater generation and reliance on fossil fuels for energy production necessitate sustainable treatment and energy recovery solutions. This study explores supercritical water gasification (SCWG) of sewage sludge from municipal wastewater as a hydrogen production pathway, focusing on the role of alkali catalysts (KOH, K₂CO₃, Na₂CO₃). The effects of temperature (450–550°C), reaction time (5–30 min), and catalyst type on gas yield and efficiency were analyzed. At 550°C, the highest carbon efficiency (61 %), gas efficiency (69 %), and hydrogen yield (41 mol/kg) were observed. After 30 min, the gas composition reached H₂ (58 %), CO₂ (26 %), CH₄ (11.7 %), and CO (4 %). Among catalysts, Na₂CO₃ exhibited superior H₂ yield (29 mol/kg), carbon efficiency (58 %), and gas efficiency (51 %). This study highlights SCWG as a viable technology for hydrogen-rich gas production, contributing to sustainable energy solutions and wastewater valorization.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103232"},"PeriodicalIF":8.4,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217712","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}

引用次数: 0

Adaptabilities of promoters in hydrate-based CO2 capture from simulated flue gases with high-temperature water vapor 促进剂在含高温水蒸气的模拟烟气中水合物基CO2捕集中的适应性

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-29 DOI: 10.1016/j.jcou.2025.103231

Peng Zhang , Xu Ma , Xudong Che , Na Yin , Yulu Wang , Lianhai Zhang , Yingmei Wang , Xuemin Zhang , Jing Zhan , Qingbai Wu , Shuanshi Fan

Besides CO₂/N₂ mixed gases, actual flue gases also contain high-temperature water vapor exceeding 100 °C. For the hydrate-based CO₂ capture technology from flue gases, except for conventional hydrate formation promoter sodium dodecyl sulfate (SDS), another eco-friendly and high-efficient L-methionine (L-Met) recently emerges, both with great application potential. By using two liquid-injecting modes, three liquids with both 640 and 160 ml volumes of pure water and solutions of two promoters were heated to 110 °C and then injected inside a reactor containing mixed gases to form CO₂ hydrates. Specific adaptabilities and accelerating mechanisms of two promoters were then investigated under high-temperature water vapor scenario. The results indicate that both 0.1 and 1.0 wt% concentrations of promoters embody more significant accelerating effects on hydrate formation than pure water, and the promoter with a concentration of 0.1 wt% has a better effect. Considering the nozzle blockage and promotion efficiency, SDS is more suitable for 0.8 mm nozzles, and L-Met is more suitable for 0.1 mm nozzles. In terms of final averaged water conversion ratios to hydrate, 1.0 wt% SDS appears higher adaptability to 640 ml liquids and 0.1 wt% L-Met to 160 ml ones. The specific acting extent of SDS appears deeper than that of L-Met and the hydrate formed using SDS has coarse-grained morphology and that using L-Met the spherical one. This implies during hydrate formations by using SDS, some liquid water might be conserved inside the capillary pores acting as the water-source to foster continuous hydrate growth; for using L-Met, hydrate formation can absorb some liquid water from a relatively large distance through mobilization behavior of liquid water. This study provides some reference for future industrial-scale application of hydrate-based decarbonization technology from flue gases, especially under high-temperature water vapor scenario.

除了CO2/N2混合气体外，实际烟气中还含有超过100°C的高温水蒸气。在基于水合物的烟气CO2捕集技术中，除了传统的水合物形成促进剂十二烷基硫酸钠（SDS）外，最近又出现了一种环保高效的l -蛋氨酸（L-Met），两者都具有很大的应用潜力。采用两种注液方式，将体积分别为640和160 ml的纯水和两种促进剂溶液的三种液体加热至110℃，注入含有混合气体的反应器中形成CO2水合物。研究了两种促进剂在高温水蒸气环境下的具体适应性和加速机理。结果表明，与纯水相比，0.1和1.0 wt%浓度的促进剂对水合物形成的加速作用更显著，且0.1 wt%浓度的促进剂效果更好。考虑喷嘴堵塞和促进效率，SDS更适合0.8 mm喷嘴，L-Met更适合0.1 mm喷嘴。就最终平均水与水合物的转化率而言，1.0 wt% SDS对640 ml液体的适应性更高，0.1 wt% L-Met对160 ml液体的适应性更高。SDS比L-Met的比作用程度更深，SDS形成的水合物晶粒较粗，L-Met形成的水合物为球形。这意味着在SDS水合物形成过程中，一些液态水可能在毛细管孔内作为水源保存，从而促进水合物的持续生长；对于L-Met，水合物形成可以通过液态水的动员行为，从较远的距离吸收部分液态水。该研究为未来烟气水合物脱碳技术的工业规模应用，特别是高温水蒸气场景下的脱碳技术提供了一定的参考。

{"title":"Adaptabilities of promoters in hydrate-based CO2 capture from simulated flue gases with high-temperature water vapor","authors":"Peng Zhang , Xu Ma , Xudong Che , Na Yin , Yulu Wang , Lianhai Zhang , Yingmei Wang , Xuemin Zhang , Jing Zhan , Qingbai Wu , Shuanshi Fan","doi":"10.1016/j.jcou.2025.103231","DOIUrl":"10.1016/j.jcou.2025.103231","url":null,"abstract":"<div><div>Besides CO<sub>2</sub>/N<sub>2</sub> mixed gases, actual flue gases also contain high-temperature water vapor exceeding 100 °C. For the hydrate-based CO<sub>2</sub> capture technology from flue gases, except for conventional hydrate formation promoter sodium dodecyl sulfate (SDS), another eco-friendly and high-efficient L-methionine (L-Met) recently emerges, both with great application potential. By using two liquid-injecting modes, three liquids with both 640 and 160 ml volumes of pure water and solutions of two promoters were heated to 110 °C and then injected inside a reactor containing mixed gases to form CO<sub>2</sub> hydrates. Specific adaptabilities and accelerating mechanisms of two promoters were then investigated under high-temperature water vapor scenario. The results indicate that both 0.1 and 1.0 wt% concentrations of promoters embody more significant accelerating effects on hydrate formation than pure water, and the promoter with a concentration of 0.1 wt% has a better effect. Considering the nozzle blockage and promotion efficiency, SDS is more suitable for 0.8 mm nozzles, and L-Met is more suitable for 0.1 mm nozzles. In terms of final averaged water conversion ratios to hydrate, 1.0 wt% SDS appears higher adaptability to 640 ml liquids and 0.1 wt% L-Met to 160 ml ones. The specific acting extent of SDS appears deeper than that of L-Met and the hydrate formed using SDS has coarse-grained morphology and that using L-Met the spherical one. This implies during hydrate formations by using SDS, some liquid water might be conserved inside the capillary pores acting as the water-source to foster continuous hydrate growth; for using L-Met, hydrate formation can absorb some liquid water from a relatively large distance through mobilization behavior of liquid water. This study provides some reference for future industrial-scale application of hydrate-based decarbonization technology from flue gases, especially under high-temperature water vapor scenario.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103231"},"PeriodicalIF":8.4,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145217713","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}

引用次数: 0

Thermodynamic analysis of CO2 methanation for power-to-gas applications: Impact of in-situ water removal on performances and heat release 动力制气应用中CO2甲烷化的热力学分析：原位除水对性能和热释放的影响

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-19 DOI: 10.1016/j.jcou.2025.103226

S.G. Acierno, C. Finelli, A. Lancia, A. Erto

This study presents a comprehensive thermodynamic analysis of CO₂ methanation, aimed at identifying optimal operating conditions for a reaction governed by a complex network. Simulations were performed in Aspen Plus® using Gibbs free energy minimization. Key variables were systematically investigated, including temperature (200–500 °C), pressure (1, 5, 10 and 30 atm), and H_2/CO₂ molar ratio (2:1, 4:1, 6:1). A special attention is given to selective water removal, analyzed across a full range (0–100 %) to simulate sorption-enhanced and membrane reactor systems. For these scenarios, the H_2/CO₂ ratio was fixed at 4:1 to reflect typical conditions. Given the exothermic nature of CO₂ hydrogenation, a thermal analysis was also performed to estimate heat release and assess the feasibility of thermoneutral operation. This was evaluated over an extended temperature range (200–700 °C) and the same pressures and feed ratios, providing insights into energy efficiency and operational stability.

Results show that water removal strongly shifts the thermodynamic equilibrium, significantly increasing CO₂ conversion and CH₄ selectivity up to a critical point, beyond which coke formation becomes favorable. The location of this optimum is highly sensitive to temperature and pressure, highlighting the need for strict operational control. Corresponding variations in the reaction heat profile further emphasize these dependencies. Overall, this work offers a detailed thermodynamic perspective on a kinetically complex system, identifies favorable operating windows and highlights process limitations. These findings complement existing literature and provide valuable guidance for the design and optimization of CO₂ methanation technologies.

本研究对二氧化碳甲烷化进行了全面的热力学分析，旨在确定由复杂网络控制的反应的最佳操作条件。在Aspen Plus®中使用吉布斯自由能最小化进行模拟。系统地研究了关键变量，包括温度（200-500°C），压力（1,5,10和30 atm）和H2/CO2摩尔比（2:1,4:1,6:1）。特别关注选择性除水，在全范围内（0-100 %）进行分析，以模拟吸附增强和膜反应器系统。对于这些场景，H2/CO2的比例固定为4:1，以反映典型情况。考虑到CO2加氢的放热性质，还进行了热分析，以估计热量释放并评估热中性操作的可行性。在更大的温度范围（200-700°C）、相同的压力和进料比下进行了评估，从而深入了解了能源效率和运行稳定性。结果表明，脱水强烈地改变了热力学平衡，显著提高了CO2转化率和CH4选择性，达到一个临界点，超过这个临界点就有利于焦炭的形成。该最佳位置对温度和压力高度敏感，因此需要严格的操作控制。反应热分布的相应变化进一步强调了这些相关性。总的来说，这项工作为动力学复杂系统提供了详细的热力学视角，确定了有利的操作窗口，并突出了过程限制。这些发现补充了现有文献，为CO2甲烷化技术的设计和优化提供了有价值的指导。

{"title":"Thermodynamic analysis of CO2 methanation for power-to-gas applications: Impact of in-situ water removal on performances and heat release","authors":"S.G. Acierno, C. Finelli, A. Lancia, A. Erto","doi":"10.1016/j.jcou.2025.103226","DOIUrl":"10.1016/j.jcou.2025.103226","url":null,"abstract":"<div><div>This study presents a comprehensive thermodynamic analysis of CO₂ methanation, aimed at identifying optimal operating conditions for a reaction governed by a complex network. Simulations were performed in Aspen Plus® using Gibbs free energy minimization. Key variables were systematically investigated, including temperature (200–500 °C), pressure (1, 5, 10 and 30 atm), and H<sub>2/</sub>CO<sub>2</sub> molar ratio (2:1, 4:1, 6:1). A special attention is given to selective water removal, analyzed across a full range (0–100 %) to simulate sorption-enhanced and membrane reactor systems. For these scenarios, the H<sub>2/</sub>CO<sub>2</sub> ratio was fixed at 4:1 to reflect typical conditions. Given the exothermic nature of CO<sub>2</sub> hydrogenation, a thermal analysis was also performed to estimate heat release and assess the feasibility of thermoneutral operation. This was evaluated over an extended temperature range (200–700 °C) and the same pressures and feed ratios, providing insights into energy efficiency and operational stability.</div><div>Results show that water removal strongly shifts the thermodynamic equilibrium, significantly increasing CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity up to a critical point, beyond which coke formation becomes favorable. The location of this optimum is highly sensitive to temperature and pressure, highlighting the need for strict operational control. Corresponding variations in the reaction heat profile further emphasize these dependencies. Overall, this work offers a detailed thermodynamic perspective on a kinetically complex system, identifies favorable operating windows and highlights process limitations. These findings complement existing literature and provide valuable guidance for the design and optimization of CO<sub>2</sub> methanation technologies.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103226"},"PeriodicalIF":8.4,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145098247","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}

引用次数: 0

Metal-free conversion of CO2 to non-isocyanate polyurethane for solid amine sorbent pellets design for CO2 capture 无金属二氧化碳转化为非异氰酸酯聚氨酯固体胺吸附剂颗粒设计的二氧化碳捕获

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-19 DOI: 10.1016/j.jcou.2025.103228

Faranak Heshmatnia, Zahra Eshaghi Gorji, Nguyan Gia Huy, Baljeet Singh, Timo Repo

Green synthesis of non-isocyanate polyurethanes (NIPUs) has attracted considerable interest as an eco-friendly alternative to traditional isocyanate-based routes. In this work, a metal-free catalytic system based on cetyltrimethylammonium bromide (CTAB) was used to transform polyfunctional epoxides into cyclic carbonates with more than 90 % conversion, which can act as key monomer precursors for NIPU formation. Furthermore, the performance of this metal-free catalyst was evaluated in a one-pot process that directly couples epoxides, CO₂ and diamine to yield NIPUs, thereby demonstrating a sustainable strategy for NIPU synthesis that leverages benign catalytic conditions and CO₂ fixation. The synthesized NIPU was explored as a binder to produce shaped solid amine sorbents for CO₂ capture using a 15 % CO₂ stream, with the resulting hollow pellets exhibiting a carbon capture capacity of 29.5 mg/g.

绿色合成非异氰酸酯聚氨酯（nipu）作为传统的基于异氰酸酯的路线的环保替代品引起了相当大的兴趣。本研究利用基于十六烷基三甲基溴化铵（CTAB）的无金属催化体系将多官能团环氧化物转化为环状碳酸盐，转化率超过90% %，可作为NIPU形成的关键单体前体。此外，该无金属催化剂的性能在一锅工艺中进行了评估，该工艺直接将环氧化物，CO 2和二胺偶联产生NIPU，从而证明了利用良性催化条件和CO 2固定来合成NIPU的可持续策略。研究了合成的NIPU作为粘合剂，使用15 % CO2流生产用于CO2捕获的成型固体胺吸附剂，所得中空颗粒的碳捕获能力为29.5 mg/g。

引用次数: 0

Ceria-doped UiO-66-derived carbon–zirconia supported vanadium catalysts for CO2-ODHP: Synergistic effects of MSI tuning, oxygen vacancies, and spillover behavior 二氧化硅掺杂uio -66衍生碳-氧化锆负载的CO2-ODHP钒催化剂：MSI调整、氧空位和溢出行为的协同效应

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-19 DOI: 10.1016/j.jcou.2025.103229

Zahra Mokhtari, Jafar Towfighi Darian, Masoud Safari Yazd

In this study, a series of zirconia-supported vanadium oxide catalysts—VZ (V₂O₅@ZrO₂), VZC (V₂O₅@ZrO₂/C, UiO-66-derived), and Ce-VZC (Ce-doped-V₂O₅@ZrO₂/C)—were synthesized and systematically evaluated for the CO₂-assisted oxidative dehydrogenation of propane (ODHP). The incorporation of a carbonaceous framework derived from UiO-66 and the strategic doping of ceria were employed to optimize metal-support interactions (MSI), enhance oxygen vacancy formation, and promote the spillover of key intermediates. A comprehensive characterization strategy—including XRD, FT-IR, HR-XPS, FE-SEM/EDS, BET, H₂-TPR, and H₂/CO₂-TPD—combined with DFT calculations was undertaken to correlate structure–property–performance relationships. The results reveal that Ce-VZC exhibited the highest surface basicity, active site dispersion, reducibility, and oxygen vacancy concentration, all of which translated into superior catalytic performance and stability. DFT calculations confirmed the lowered energy barriers for propane dehydrogenation and CO₂ activation in Ce-VZC, while also demonstrating moderated MSI and longer spillover distances of H, O, and CO₂ species. Among the catalysts, Ce-VZC achieved the highest propane conversion (19.3 %) and propylene yield (13.9 %) with excellent stability over 600 min of time-on-stream. This work highlights the synergistic effect of ceria doping and carbon integration in tuning MSI, redox properties, and intermediate spillover, offering a promising route toward the rational design of high-performance ODHP catalysts.

本研究合成了一系列氧化锆负载型钒催化剂vz （V2O5@ZrO2）、VZC （V2O5@ZrO2/C， uhio -66衍生）和Ce-VZC (Ce-doped-V2O5@ZrO2/C)，并对其用于丙烷co2辅助氧化脱氢（ODHP）进行了系统评价。采用UiO-66衍生的碳质框架和铈的战略性掺杂来优化金属-支撑相互作用（MSI），增强氧空位的形成，并促进关键中间体的溢出。采用综合表征策略，包括XRD、FT-IR、HR-XPS、FE-SEM/EDS、BET、H2- tpr和H2/ co2 - tpd，并结合DFT计算来关联结构-性能-性能关系。结果表明，Ce-VZC具有最高的表面碱度、活性位点分散性、还原性和氧空位浓度，具有优异的催化性能和稳定性。DFT计算证实了Ce-VZC中丙烷脱氢和CO2活化的能量势垒降低，同时也表明了H、O和CO2物质的MSI缓和和更长的溢出距离。在催化剂中，Ce-VZC的丙烷转化率最高（19.3 %），丙烯收率最高（13.9 %），在600 min的运行时间内具有优异的稳定性。这项工作强调了铈掺杂和碳整合在调整MSI、氧化还原性能和中间溢出方面的协同作用，为合理设计高性能ODHP催化剂提供了一条有希望的途径。

{"title":"Ceria-doped UiO-66-derived carbon–zirconia supported vanadium catalysts for CO2-ODHP: Synergistic effects of MSI tuning, oxygen vacancies, and spillover behavior","authors":"Zahra Mokhtari, Jafar Towfighi Darian, Masoud Safari Yazd","doi":"10.1016/j.jcou.2025.103229","DOIUrl":"10.1016/j.jcou.2025.103229","url":null,"abstract":"<div><div>In this study, a series of zirconia-supported vanadium oxide catalysts—VZ (V<sub>2</sub>O<sub>5</sub>@ZrO<sub>2</sub>), VZC (V<sub>2</sub>O<sub>5</sub>@ZrO<sub>2</sub>/C, UiO-66-derived), and Ce-VZC (Ce-doped-V<sub>2</sub>O<sub>5</sub>@ZrO<sub>2</sub>/C)—were synthesized and systematically evaluated for the CO<sub>2</sub>-assisted oxidative dehydrogenation of propane (ODHP). The incorporation of a carbonaceous framework derived from UiO-66 and the strategic doping of ceria were employed to optimize metal-support interactions (MSI), enhance oxygen vacancy formation, and promote the spillover of key intermediates. A comprehensive characterization strategy—including XRD, FT-IR, HR-XPS, FE-SEM/EDS, BET, H<sub>2</sub>-TPR, and H<sub>2</sub>/CO<sub>2</sub>-TPD—combined with DFT calculations was undertaken to correlate structure–property–performance relationships. The results reveal that Ce-VZC exhibited the highest surface basicity, active site dispersion, reducibility, and oxygen vacancy concentration, all of which translated into superior catalytic performance and stability. DFT calculations confirmed the lowered energy barriers for propane dehydrogenation and CO<sub>2</sub> activation in Ce-VZC, while also demonstrating moderated MSI and longer spillover distances of H, O, and CO<sub>2</sub> species. Among the catalysts, Ce-VZC achieved the highest propane conversion (19.3 %) and propylene yield (13.9 %) with excellent stability over 600 min of time-on-stream. This work highlights the synergistic effect of ceria doping and carbon integration in tuning MSI, redox properties, and intermediate spillover, offering a promising route toward the rational design of high-performance ODHP catalysts.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103229"},"PeriodicalIF":8.4,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145098250","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}

引用次数: 0

Paradigmatic demonstration of sonochemical carbon dioxide reduction proceeded over Cu-based catalysts 在cu基催化剂上进行了声化学二氧化碳还原的范例演示

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization

Pub Date : 2025-09-19 DOI: 10.1016/j.jcou.2025.103220

Dong Xia , Yi Qin , Yagya N. Regmi , Laurie A. King , James Kwan

Sonochemical carbon dioxide (CO₂) reduction represents a promising decarbonization technology. However, relevant studies regarding the usage of solid catalysts in sonochemical reactor are rare. Herein, we investigate four distinct highly nanostructured cuprous oxides and sulfides for sonochemical CO₂ reduction via ultrasound-induced cavitation. Specifically, we investigate Cu₂O cubes, Cu₇S₄/Cu₂O cubes, Cu₇S₄ cages and Cu₇S₄ sheets morphologies. Each nanostructure is found to produce CO and H₂ in various ratios ranging from 1.0 – 2.3. Through a systematic study, we investigate the role of different acoustic conditions on affecting CO₂ sonolysis, involving the measurements in CO₂-saturated H₂O, 5 %CO₂/Ar-saturated H₂O, N₂-saturated H₂O, 5 %CO₂/N₂-saturated H₂O and CO₂-saturated KHCO₃. We show that Cu₂O cubes have the highest CO₂-to-CO conversion (up to 4286.4 μmol·L⁻¹·g⁻¹·h⁻¹) in 5 %CO₂/Ar-saturated H₂O. In addition, the as-synthesized Cu₂O cubes exhibited promising sonochemical stability, with CO and H₂ production rates stabilizing at around 890.3 μmol·L⁻¹·g⁻¹·h⁻¹ and 966.9 μmol·L⁻¹·g⁻¹·h⁻¹, respectively. Post sonochemical analysis indicated that the Cu₂O cubes maintain relatively high CO₂-to-CO conversion, as well as their morphology. This work provides the first proof-of-concept demonstration of using inexpensive Cu-based catalysts to enable low-carbon sonochemical CO₂ reduction.

声化学二氧化碳（CO2）还原是一种很有前途的脱碳技术。然而，固体催化剂在声化学反应器中应用的相关研究很少。在此，我们研究了四种不同的高纳米结构的亚铜氧化物和硫化物，通过超声诱导空化进行声化学CO2还原。具体来说，我们研究了Cu2O立方体、Cu7S4/Cu2O立方体、Cu7S4笼和Cu7S4薄片的形貌。研究发现，每种纳米结构产生的CO和H2的比例在1.0 - 2.3之间。通过对CO2饱和H2O、5 %CO2/ ar饱和H2O、n2饱和H2O、5 %CO2/ n2饱和H2O和CO2饱和KHCO3的测量，系统地研究了不同声学条件对CO2声溶的影响。结果表明，Cu2O立方体在5 %CO2/ ar饱和水中具有最高的CO2-to- co转化率（高达4286.4 μmol·L−1·g−1·h−1）。此外，合成的Cu2O立方体具有良好的声化学稳定性，CO和H2的产率分别稳定在890.3 μmol·L−1·g−1·h−1和966.9 μmol·L−1·g−1·h−1左右。后声化学分析表明，Cu2O立方体保持了较高的CO2-to-CO转化率，其形貌也保持不变。这项工作提供了使用廉价的cu基催化剂实现低碳声化学二氧化碳还原的第一个概念验证演示。

{"title":"Paradigmatic demonstration of sonochemical carbon dioxide reduction proceeded over Cu-based catalysts","authors":"Dong Xia , Yi Qin , Yagya N. Regmi , Laurie A. King , James Kwan","doi":"10.1016/j.jcou.2025.103220","DOIUrl":"10.1016/j.jcou.2025.103220","url":null,"abstract":"<div><div>Sonochemical carbon dioxide (CO<sub>2</sub>) reduction represents a promising decarbonization technology. However, relevant studies regarding the usage of solid catalysts in sonochemical reactor are rare. Herein, we investigate four distinct highly nanostructured cuprous oxides and sulfides for sonochemical CO<sub>2</sub> reduction via ultrasound-induced cavitation. Specifically, we investigate Cu<sub>2</sub>O cubes, Cu<sub>7</sub>S<sub>4</sub>/Cu<sub>2</sub>O cubes, Cu<sub>7</sub>S<sub>4</sub> cages and Cu<sub>7</sub>S<sub>4</sub> sheets morphologies. Each nanostructure is found to produce CO and H<sub>2</sub> in various ratios ranging from 1.0 – 2.3. Through a systematic study, we investigate the role of different acoustic conditions on affecting CO<sub>2</sub> sonolysis, involving the measurements in CO<sub>2</sub>-saturated H<sub>2</sub>O, 5 %CO<sub>2</sub>/Ar-saturated H<sub>2</sub>O, N<sub>2</sub>-saturated H<sub>2</sub>O, 5 %CO<sub>2</sub>/N<sub>2</sub>-saturated H<sub>2</sub>O and CO<sub>2</sub>-saturated KHCO<sub>3</sub>. We show that Cu<sub>2</sub>O cubes have the highest CO<sub>2</sub>-to-CO conversion (up to 4286.4 μmol·L<sup>−1</sup>·g<sup>−1</sup>·h<sup>−1</sup>) in 5 %CO<sub>2</sub>/Ar-saturated H<sub>2</sub>O. In addition, the as-synthesized Cu<sub>2</sub>O cubes exhibited promising sonochemical stability, with CO and H<sub>2</sub> production rates stabilizing at around 890.3 μmol·L<sup>−1</sup>·g<sup>−1</sup>·h<sup>−1</sup> and 966.9 μmol·L<sup>−1</sup>·g<sup>−1</sup>·h<sup>−1</sup>, respectively. Post sonochemical analysis indicated that the Cu<sub>2</sub>O cubes maintain relatively high CO<sub>2</sub>-to-CO conversion, as well as their morphology. This work provides the first proof-of-concept demonstration of using inexpensive Cu-based catalysts to enable low-carbon sonochemical CO<sub>2</sub> reduction.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103220"},"PeriodicalIF":8.4,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145098248","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}

引用次数: 0