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Bioinspired porous cementitious materials for CO₂ capture: A critical review of accelerated carbonation strategies 生物激发多孔胶凝材料用于CO₂捕获:加速碳化策略的重要回顾
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-01-06 DOI: 10.1016/j.jcou.2025.103299
Joaquim Constantino , João Castro-Gomes , Maria Inês Alves Vicente
This critical review presents a comprehensive synthesis of recent advances in the development of bioinspired porous cementitious materials for enhanced CO₂ capture via accelerated carbonation. Addressing the urgent demand for sustainable construction solutions, the study consolidates current literature on pore structure optimisation including pore size, distribution, interconnectivity, and specific surface area and their influence on carbonation kinetics and sequestration efficiency. Inspired by hierarchical biological systems such as corals, mollusc shells, and marine sponges, the review explores the translation of structural and functional principles into cementitious matrices. A comparative analysis of key accelerated carbonation strategies standard curing, pressurised systems, flow-through techniques, and water CO₂ cooperative processes is provided, highlighting their mechanistic bases, process parameters, and industrial scalability. The technological readiness and real-world applicability of CO₂-mineralising concrete are assessed through selected industrial case studies, contextualised within circular economy and carbon neutrality frameworks. Finally, the review identifies critical knowledge gaps and outlines future research directions to advance next-generation low-carbon cementitious materials that integrate mechanical performance, tailored porosity, and environmental functionality.
这篇重要的综述介绍了生物激发多孔胶凝材料的发展的最新进展,通过加速碳化来增强二氧化碳捕获。为了解决对可持续建筑解决方案的迫切需求,该研究整合了目前关于孔隙结构优化的文献,包括孔隙大小、分布、连通性、比表面积及其对碳化动力学和封存效率的影响。受珊瑚、软体动物壳和海洋海绵等分层生物系统的启发,本文探讨了将结构和功能原理转化为胶凝基质的方法。对关键的加速碳化策略进行了比较分析,标准固化、加压系统、流动技术和水- CO - 2协同工艺,强调了它们的机理基础、工艺参数和工业可扩展性。通过选定的工业案例研究,在循环经济和碳中和框架的背景下,评估二氧化碳矿化混凝土的技术准备程度和现实世界的适用性。最后,该综述确定了关键的知识空白,并概述了未来的研究方向,以推进下一代低碳胶凝材料,该材料集机械性能、定制孔隙度和环境功能于一体。
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引用次数: 0
Toward sustainable catalysis: Anion-engineered metal-/halogen-free catalysts for efficient chemical fixation of low concentration CO2 迈向可持续催化:阴离子工程的无金属/无卤素催化剂,用于低浓度二氧化碳的有效化学固定
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-01-01 DOI: 10.1016/j.jcou.2025.103308
Zhilei Dai , Jing Zhang , Yiling Tong , Ning Zhou , Songyao Liu , Zhifeng Dai , Yubing Xiong
The efficient conversion of atmospheric CO2 into high value-added chemicals remains a persistent challenge. In this study, a heterogeneous catalyst PDxBpyOH with both metal-free and halogen-free properties and nucleophilic hydroxyl sites was developed for the cycloaddition reaction of CO2 with epoxides. This catalyst was constructed by incorporating a bipyridine complex and a imidazolium salt into an organic polymer matrix, followed by anion exchange. The porosity structure of these catalysts were optimized by tuning the crosslinker DVB ratio (x = 0, 2, 3, 4). A series of characterizations confirmed that it had a hierarchical micro-mesoporous structure, and the specific surface area regulated by DVB improved the physical adsorption capacity of CO2. Under the optimal conditions (80 mg catalyst, 60 °C, 1 atm CO2, 48 h), PD2BpyOH achieved 89 % conversion of epichlorohydrin. Furthermore, it maintained 85 % conversion in 96 h under simulated industrial flue gas (15 % CO2/85 % N2), demonstrating robust recyclability and activity for various epoxides. This catalytic system provides a new metal-free and halogen-free heterogeneous catalytic strategy for the utilization of low-concentration CO2.
将大气中的二氧化碳有效地转化为高附加值的化学品仍然是一个持久的挑战。本研究开发了一种具有无金属、无卤素、亲核羟基的非均相催化剂PDxBpyOH,用于CO2与环氧化物的环加成反应。该催化剂是通过将联吡啶配合物和咪唑盐结合到有机聚合物基质中,然后进行阴离子交换而构建的。通过调节交联剂DVB的比例(x = 0,2,3,4),优化了催化剂的孔隙结构。一系列表征证实了其具有层次微介孔结构,且DVB调控的比表面积提高了其对CO2的物理吸附能力。在最佳条件下(80 mg催化剂,60°C, 1 atm CO2, 48 h), PD2BpyOH的环氧氯丙烷转化率为89 %。此外,在模拟工业烟气(15 % CO2/85 % N2)下,它在96 h内保持85 %的转化率,显示出对各种环氧化物的强大可回收性和活性。该催化体系为低浓度CO2的利用提供了一种新的无金属、无卤素的非均相催化策略。
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引用次数: 0
Techno-economic analysis of carbon-based additives and process optimization for enhanced hydrogen production in integrated pyrolysis/gasification and carbon capture systems 碳基添加剂的技术经济分析和工艺优化,以提高综合热解/气化和碳捕集系统的氢气产量
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-01-01 DOI: 10.1016/j.jcou.2025.103296
Wenxin Lu , Yuxing Ding , Zhaoxi Dong , Xin Peng , Yue Chai , Dunfeng Xiao , Yurong Liu , Feng Qian , Iqbal M. Mujtaba
Overexploitation of fossil fuels leads to issues of energy security and environmental pollution. Integrating carbon capture and utilisation (CCU) with biomass and waste plastics pyrolysis/gasification offers a promising route for simultaneous hydrogen production and CO₂ mitigation. However, hydrogen yield is often limited in such integrated systems. This study developed an Aspen Plus model to evaluate the effects of carbon-based additives, steam flow rate, and reforming temperature on H₂ production and process economics. Results show that application of CCU to pyrolysis/gasification decreases H2 yield from 5.28 to 4.61 mol/hr, and only a small quantity of carbon additives (0.13 additives-to-feed ratio) can restore the H2 yield to 5.33 mol/hr, which is higher than the original level of 5.28 mol/hr when no CCU is applied. An optimal steam flowrate is required to balance enhanced H₂ generation against the undesired increase in CO₂ formation that may offset the benefit of carbon capture. 600 °C is identified as the optimal temperature with the highest H2 yield. Economic analysis also indicates the levelized cost of hydrogen (LCOH) at different operating conditions. A multi-objective optimisation was also performed to find an optimal operating point at 1.50 g/min carbon addition, 8.75 g/min steam flowrate, and 669.92 °C reforming temperature, corresponding to an H₂ yield of 14.04 mol/h and an LCOH of 3.49 $/kg. The findings provide quantitative guidance for optimising integrated pyrolysis/gasification–CCU systems toward industrial deployment.
化石燃料的过度开采导致能源安全和环境污染问题。将碳捕获和利用(CCU)与生物质和废塑料热解/气化相结合,为同时生产氢气和减少CO 2提供了一条有前途的途径。然而,在这样的集成系统中,氢的产率通常是有限的。本研究开发了一个Aspen Plus模型来评估碳基添加剂、蒸汽流量和重整温度对H₂产量和工艺经济的影响。结果表明,在热解/气化过程中使用CCU使H2产率从5.28降低到4.61 mol/hr,而少量添加碳添加剂(料料比0.13)可使H2产率恢复到5.33 mol/hr,高于未添加CCU时的5.28 mol/hr。需要一个最佳的蒸汽流量来平衡增强的H 2生成与不希望的CO 2生成的增加,CO 2生成可能抵消碳捕获的好处。600℃是H2产率最高的最佳温度。经济分析还指出了不同工况下氢气的平准化成本。在碳添加量为1.50 g/min、蒸汽流量为8.75 g/min、重整温度为669.92℃的条件下进行了多目标优化,得到的H₂产率为14.04 mol/ H, LCOH为3.49美元/kg。研究结果为优化工业部署的热解/气化- ccu集成系统提供了定量指导。
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引用次数: 0
Selective CO2 adsorption over alkali metal cation-exchanged UZM-9 zeolites 碱金属阳离子交换UZM-9沸石对CO2的选择性吸附
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-01-01 DOI: 10.1016/j.jcou.2025.103305
Jakub Halamek , Martin Kubů , Branislav Koreň , Jiří Čejka , Jan Valenta , Roman Bulánek
Adsorption on zeolites reduces CO2 emissions and cuts the energy costs of processing gas mixtures, such as natural gas, biogas, and landfill gas (CO2/CH4 of various concentrations). Among zeolite frameworks, LTA stands out for its CO2 adsorption and/or separation potential, particularly the Na-LTA zeolite with a Si/Al ratio of ∼5. However, the impact of different cations on the separation efficiency of this system remains unknown. In this study, we tested various alkali-metal-exchanged UZM-9 zeolites (Si/Al = 4.5) for their selective adsorption of CO2 over CH4. K+-exchanged UZM-9 reached the highest CO2 affinity, isosteric heat of adsorption, and selectivity, outperforming more commonly used Na+ forms. This enhanced performance likely stems from the predominant location of K+ in the 8-ring window, which fosters strong CO2 interactions, potentially via bridging CO2 species. Due to partial pore blocking, the total uptake may decrease slightly, but the K-UZM-9 system effectively balances CO2/CH4 selectivity and adsorption capacity. Therefore, K-UZM-9 emerges as a promising adsorbent for energy-efficient gas separation and carbon capture applications.
沸石上的吸附减少了二氧化碳的排放,并降低了处理天然气、沼气和垃圾填埋气(不同浓度的CO2/CH4)等混合气体的能源成本。在沸石框架中,LTA因其CO2吸附和/或分离潜力而脱颖而出,特别是Si/Al比为~ 5的Na-LTA沸石。然而,不同阳离子对该体系分离效率的影响尚不清楚。在这项研究中,我们测试了各种碱金属交换的UZM-9沸石(Si/Al = 4.5)对CO2在CH4上的选择性吸附。K+交换的UZM-9具有最高的CO2亲和力、等容吸附热和选择性,优于更常用的Na+形式。这种增强的性能可能源于K+在8环窗口中的主要位置,这可能通过桥接CO2种促进了强烈的CO2相互作用。由于部分孔隙堵塞,总吸收率可能会略有下降,但K-UZM-9体系有效地平衡了CO2/CH4的选择性和吸附能力。因此,K-UZM-9成为一种有前途的吸附剂,用于节能气体分离和碳捕获应用。
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引用次数: 0
Multi-walled carbon nanotube–integrated Cu–ZnO/Al2O3 catalysts: A hybrid support strategy for structural modulation and efficient CO2 hydrogenation to methanol 多壁碳纳米管集成Cu-ZnO /Al2O3催化剂:结构调制和高效CO2加氢制甲醇的混合支持策略
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-01-01 DOI: 10.1016/j.jcou.2025.103306
Esmaeil GhasemiKafrudi , Navid Mostoufi , Alimorad Rashidi , Reza Zarghami
A novel hybrid Cu(30 %)-ZnO(41 %)/Al2O3/MWCNT catalyst was developed to enhance hydrogenation of CO2 to methanol. Multi-walled carbon nanotubes (MWCNTs) were functionalized and incorporated into catalysts with varying carbon contents (0–12 wt%) via co-precipitation. The catalysts were characterized using standard techniques, including XRD, FESEM, TEM, FTIR, Raman spectroscopy, TPR, and CO2-TPD, to evaluate their structural, morphological, and chemical properties. The results demonstrated that MWCNTs integration significantly improved metal dispersion, prevented particle agglomeration, and enhanced CO2 adsorption. The experiments showed that, among all catalyst formulations and the two industrial reference samples, the catalyst with 8 wt% MWCNTs exhibited the highest methanol yield (13.4 %) and a 25 % increase in space–time yield compared to the MWCNT-free catalyst (11.0 %). Furthermore, the catalyst demonstrated excellent long-term stability, preserving its structural integrity and catalytic performance over 60 h of continuous operation. The implementation of this hybrid catalyst as a replacement for the MWCNT-free formulation in the CO2 hydrogenation process resulted in a 6.1 % reduction in total energy demand, which consequently led to a 7.3 % decrease in greenhouse gas emissions (32.5 kg CO2/ton MeOH). These findings confirm that incorporation of MWCNTs constitutes an effective hybrid-support strategy for structural modulation and performance enhancement in CO2 hydrogenation catalysts.
研制了一种新型Cu(30 %)-ZnO(41 %)/Al2O3/MWCNT杂化催化剂,以促进CO2加氢制甲醇。通过共沉淀法将多壁碳纳米管(MWCNTs)功能化并掺入不同碳含量(0-12 wt%)的催化剂中。采用XRD、FESEM、TEM、FTIR、拉曼光谱、TPR和CO2-TPD等标准技术对催化剂进行表征,评价催化剂的结构、形态和化学性质。结果表明,MWCNTs的整合显著改善了金属的分散,防止了颗粒团聚,并增强了CO2的吸附。实验表明,在所有催化剂配方和两种工业参考样品中,与不含mwcnt的催化剂(11.0 %)相比,含8 wt% mwcnt的催化剂甲醇收率最高(13.4 %),空时收率提高了25 %。此外,该催化剂表现出优异的长期稳定性,在60 h的连续运行中保持其结构完整性和催化性能。在二氧化碳加氢过程中,使用这种混合催化剂替代无mwcnt配方,总能源需求减少了6.1 %,从而导致温室气体排放量减少了7.3 %(32.5 kg CO2/吨MeOH)。这些发现证实,在CO2加氢催化剂中加入MWCNTs是一种有效的混合负载策略,可用于结构调节和性能增强。
{"title":"Multi-walled carbon nanotube–integrated Cu–ZnO/Al2O3 catalysts: A hybrid support strategy for structural modulation and efficient CO2 hydrogenation to methanol","authors":"Esmaeil GhasemiKafrudi ,&nbsp;Navid Mostoufi ,&nbsp;Alimorad Rashidi ,&nbsp;Reza Zarghami","doi":"10.1016/j.jcou.2025.103306","DOIUrl":"10.1016/j.jcou.2025.103306","url":null,"abstract":"<div><div>A novel hybrid Cu(30 %)-ZnO(41 %)/Al<sub>2</sub>O<sub>3</sub>/MWCNT catalyst was developed to enhance hydrogenation of CO<sub>2</sub> to methanol. Multi-walled carbon nanotubes (MWCNTs) were functionalized and incorporated into catalysts with varying carbon contents (0–12 wt%) via co-precipitation. The catalysts were characterized using standard techniques, including XRD, FESEM, TEM, FTIR, Raman spectroscopy, TPR, and CO<sub>2</sub>-TPD, to evaluate their structural, morphological, and chemical properties. The results demonstrated that MWCNTs integration significantly improved metal dispersion, prevented particle agglomeration, and enhanced CO<sub>2</sub> adsorption. The experiments showed that, among all catalyst formulations and the two industrial reference samples, the catalyst with 8 wt% MWCNTs exhibited the highest methanol yield (13.4 %) and a 25 % increase in space–time yield compared to the MWCNT-free catalyst (11.0 %). Furthermore, the catalyst demonstrated excellent long-term stability, preserving its structural integrity and catalytic performance over 60 h of continuous operation. The implementation of this hybrid catalyst as a replacement for the MWCNT-free formulation in the CO<sub>2</sub> hydrogenation process resulted in a 6.1 % reduction in total energy demand, which consequently led to a 7.3 % decrease in greenhouse gas emissions (32.5 kg CO<sub>2</sub>/ton MeOH). These findings confirm that incorporation of MWCNTs constitutes an effective hybrid-support strategy for structural modulation and performance enhancement in CO<sub>2</sub> hydrogenation catalysts.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"103 ","pages":"Article 103306"},"PeriodicalIF":8.4,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145938413","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
Sensitivity analysis of the H2S breakthrough curve in a column packed with type 13X zeolite: Parametric study of pressure swing adsorption process for CO2 separation and biomethane production 13X型沸石填料柱中H2S突破曲线的敏感性分析:变压吸附CO2分离和生物甲烷生产过程的参数研究
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1016/j.jcou.2025.103304
Jesse Y. Rumbo-Morales , Felipe D.J. Sorcia-Vázquez , Gerardo Ortiz Torres , Alexis U. Salas Villalobos , Carlos Alberto Torres-Cantero , Manuela Calixto-Rodriguez , Antonio Márquez Rosales , Mayra G. Mena-Enriquez , Mario A. Juarez , Alan Cruz Rojas , Miguel Beltrán-Escobar , Jesús E. Valdez-Resendiz
Biomethane is a renewable energy source obtained by purifying biogas, removing impurities such as H2S and CO2. The removal of H2S is essential due to its toxicity and corrosiveness, protecting equipment and improving process efficiency. Pressure Swing Adsorption (PSA) is used to separate CO2, which produces a methane-rich gas. This process is efficient, clean, and key to utilizing biogas as a substitute for natural gas. This study aims to perform a sensitivity analysis on the H2S removal stage using a packed column with 13X zeolite, and to conduct a parametric study of the PSA process to identify input variables that significantly affect CO2 adsorption and achieve high-purity biomethane (above 99%). Comparative results showed that a pressure of 10 bar at a temperature of 298 K achieved the lowest H2S removal (1100 ppm), in a period of 4000 s; however, the highest H2S removal was achieved at 2 bar and 440 K, reaching 1500 ppm removal in 900 s. In the case of CO2 retention, the input variables that have the least effect on biomethane purity and that present the least adsorption of CO2 were the feed pressure and purge pressure variables, achieving a biomethane purity between the ranges of 97.53 % and 98.86 % and adsorbing between 0.35 to 0.38 molar fraction using only 0.6 m of the total bed length. On the other hand, the input variables that achieved the highest adsorption capacity (0.5 molar fraction) were temperature and composition, achieving to use the longest length of the packed bed (0.8 m) and reaching a biomethane purity of 99.05%, which meets established international criteria to be used as biofuel.
生物甲烷是一种可再生能源,通过净化沼气,去除H2S和CO2等杂质而获得。由于其毒性和腐蚀性,清除H2S对于保护设备和提高工艺效率至关重要。变压吸附(PSA)用于分离二氧化碳,从而产生一种富含甲烷的气体。这一过程高效、清洁,是利用沼气替代天然气的关键。本研究旨在利用13X沸石填充柱对H2S去除阶段进行敏感性分析,并对PSA过程进行参数化研究,以确定显著影响CO2吸附的输入变量,并获得高纯度的生物甲烷(99%以上)。对比结果表明,在298 K的温度下,10 bar的压力在4000 s的时间内达到了最低的H2S去除率(1100 ppm);然而,在2bar和440k条件下,H2S去除率最高,在900s内达到1500ppm。在CO2滞留的情况下,对生物甲烷纯度影响最小的输入变量和对CO2的吸附最少的输入变量是进料压力和吹扫压力变量,实现生物甲烷纯度在97.53%到98.86%之间,吸附在0.35到0.38摩尔分数之间,仅使用0.6 m的总床长。另一方面,获得最高吸附容量(0.5摩尔分数)的输入变量是温度和成分,实现了使用最长的填充床长度(0.8 m),并达到99.05%的生物甲烷纯度,符合国际标准,用于生物燃料。
{"title":"Sensitivity analysis of the H2S breakthrough curve in a column packed with type 13X zeolite: Parametric study of pressure swing adsorption process for CO2 separation and biomethane production","authors":"Jesse Y. Rumbo-Morales ,&nbsp;Felipe D.J. Sorcia-Vázquez ,&nbsp;Gerardo Ortiz Torres ,&nbsp;Alexis U. Salas Villalobos ,&nbsp;Carlos Alberto Torres-Cantero ,&nbsp;Manuela Calixto-Rodriguez ,&nbsp;Antonio Márquez Rosales ,&nbsp;Mayra G. Mena-Enriquez ,&nbsp;Mario A. Juarez ,&nbsp;Alan Cruz Rojas ,&nbsp;Miguel Beltrán-Escobar ,&nbsp;Jesús E. Valdez-Resendiz","doi":"10.1016/j.jcou.2025.103304","DOIUrl":"10.1016/j.jcou.2025.103304","url":null,"abstract":"<div><div>Biomethane is a renewable energy source obtained by purifying biogas, removing impurities such as H<sub>2</sub>S and CO<sub>2</sub>. The removal of H<sub>2</sub>S is essential due to its toxicity and corrosiveness, protecting equipment and improving process efficiency. Pressure Swing Adsorption (PSA) is used to separate CO<sub>2</sub>, which produces a methane-rich gas. This process is efficient, clean, and key to utilizing biogas as a substitute for natural gas. This study aims to perform a sensitivity analysis on the H<sub>2</sub>S removal stage using a packed column with 13X zeolite, and to conduct a parametric study of the PSA process to identify input variables that significantly affect CO<sub>2</sub> adsorption and achieve high-purity biomethane (above 99%). Comparative results showed that a pressure of 10 <span><math><mrow><mi>b</mi><mi>a</mi><mi>r</mi></mrow></math></span> at a temperature of 298 <span><math><mi>K</mi></math></span> achieved the lowest H<sub>2</sub>S removal (1100 <span><math><mrow><mi>p</mi><mi>p</mi><mi>m</mi></mrow></math></span>), in a period of 4000 <span><math><mi>s</mi></math></span>; however, the highest H<sub>2</sub>S removal was achieved at 2 <span><math><mrow><mi>b</mi><mi>a</mi><mi>r</mi></mrow></math></span> and 440 <span><math><mi>K</mi></math></span>, reaching 1500 <span><math><mrow><mi>p</mi><mi>p</mi><mi>m</mi></mrow></math></span> removal in 900 <span><math><mi>s</mi></math></span>. In the case of CO<sub>2</sub> retention, the input variables that have the least effect on biomethane purity and that present the least adsorption of CO<sub>2</sub> were the feed pressure and purge pressure variables, achieving a biomethane purity between the ranges of 97.53 % and 98.86 % and adsorbing between 0.35 to 0.38 molar fraction using only 0.6 <span><math><mi>m</mi></math></span> of the total bed length. On the other hand, the input variables that achieved the highest adsorption capacity (0.5 molar fraction) were temperature and composition, achieving to use the longest length of the packed bed (0.8 <span><math><mi>m</mi></math></span>) and reaching a biomethane purity of 99.05%, which meets established international criteria to be used as biofuel.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"103 ","pages":"Article 103304"},"PeriodicalIF":8.4,"publicationDate":"2025-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145797956","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
High-yield solar photocatalytic CO₂ conversion in dense-phase CO₂ via ZnO/CuO/Ti₃C₂ nanosheet heterojunctions with ionic liquids 通过ZnO/CuO/Ti₃C₂纳米片与离子液体异质结在致密相CO₂中高产太阳能光催化CO₂转化
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1016/j.jcou.2025.103300
Zhe Wang , Samar Al Jitan , Hassan A. Salih , Cyril Aubry , Thomas Delclos , Inas AlNashef , Khalid Al-Ali , Giovanni Palmisano
Harnessing solar energy to convert liquid carbon dioxide (CO2) into chemical fuels presents a promising solution to address both the greenhouse effect and the fossil fuel crisis. In this study, heterogeneous photocatalysts composed of zinc oxide (ZnO) nanocones and semi-hedgehog-like cupric oxide (CuO) nanoparticles were successfully synthesized via a hydrothermal treatment for efficient photocatalytic reduction of liquid CO2. To further enhance performance, two-dimensional Ti3C2 MXene nanosheets (NSs), corresponding to 5 mol% relative to ZnO, were integrated onto the composite photocatalyst surface, enhancing the specific surface area, facilitating interfacial charge transfer, and promoting the separation of photo-generated electron-hole pairs. Furthermore, 1-Ethyl-3methylimidazolium amino-acetate ionic liquid (IL) was utilized to lower the overpotential and enhance CO2 adsorption and diffusion. This led to a pronounced hydrogenation effect that significantly boosted methane yield in the photocatalytic process. As a result, the ZnO/CuO/Ti3C2 NSs/ILs heterojunction nanocomposite demonstrated significantly enhanced photocatalytic activity for dense-phase CO2 reduction compared to pristine ZnO nanoparticles. Using water as a hydrogen source, ZnO/0.5CuO/Ti3C2 NSs exhibit a very high total yield for liquid CO2 reduction (62 bar and 22 °C), reaching 136.9 mmol h⁻¹ g⁻¹ for CO and 30.2 mmol h⁻¹ g⁻¹ for CH₄ under irradiation of a Xe arc lamp. This remarkable production rate marks a significant step forward in the development of efficient CO2 reduction systems and presents a promising strategy for advancing solar-driven carbon conversion technologies.
利用太阳能将液态二氧化碳(CO2)转化为化学燃料是解决温室效应和化石燃料危机的一个有希望的解决方案。在本研究中,通过水热处理成功合成了由氧化锌纳米锥和半刺猬状氧化铜纳米锥组成的非均相光催化剂,用于高效光催化还原液态CO2。为了进一步提高性能,在复合光催化剂表面集成了二维Ti3C2 MXene纳米片(NSs),其相对ZnO的质量分数为5 mol%,从而提高了复合光催化剂的比表面积,促进了界面电荷转移,促进了光生电子-空穴对的分离。此外,利用1-乙基-3甲基咪唑氨基乙酸离子液体(IL)降低过电位,增强CO2的吸附和扩散。这导致了明显的氢化效应,显著提高了光催化过程中的甲烷产量。结果表明,ZnO/CuO/Ti3C2 NSs/ILs异质结纳米复合材料对浓相CO2还原的光催化活性明显高于原始ZnO纳米颗粒。使用水作为氢源,氧化锌/ 0.5措/ Ti3C2 NSs表现出非常高的总收率为液体二氧化碳减少(62 酒吧和22 °C),达到136.9 更易 h⁻¹ g⁻¹ CO和30.2 更易 h⁻¹ g⁻¹ 为CH₄Xe弧灯的照射下。这一惊人的生产速度标志着高效二氧化碳减排系统的发展向前迈出了重要一步,并为推进太阳能驱动的碳转换技术提供了一个有前途的战略。
{"title":"High-yield solar photocatalytic CO₂ conversion in dense-phase CO₂ via ZnO/CuO/Ti₃C₂ nanosheet heterojunctions with ionic liquids","authors":"Zhe Wang ,&nbsp;Samar Al Jitan ,&nbsp;Hassan A. Salih ,&nbsp;Cyril Aubry ,&nbsp;Thomas Delclos ,&nbsp;Inas AlNashef ,&nbsp;Khalid Al-Ali ,&nbsp;Giovanni Palmisano","doi":"10.1016/j.jcou.2025.103300","DOIUrl":"10.1016/j.jcou.2025.103300","url":null,"abstract":"<div><div>Harnessing solar energy to convert liquid carbon dioxide (CO<sub>2</sub>) into chemical fuels presents a promising solution to address both the greenhouse effect and the fossil fuel crisis. In this study, heterogeneous photocatalysts composed of zinc oxide (ZnO) nanocones and semi-hedgehog-like cupric oxide (CuO) nanoparticles were successfully synthesized via a hydrothermal treatment for efficient photocatalytic reduction of liquid CO<sub>2</sub>. To further enhance performance, two-dimensional Ti<sub>3</sub>C<sub>2</sub> MXene nanosheets (NSs), corresponding to 5 mol% relative to ZnO, were integrated onto the composite photocatalyst surface, enhancing the specific surface area, facilitating interfacial charge transfer, and promoting the separation of photo-generated electron-hole pairs. Furthermore, 1-Ethyl-3methylimidazolium amino-acetate ionic liquid (IL) was utilized to lower the overpotential and enhance CO<sub>2</sub> adsorption and diffusion. This led to a pronounced hydrogenation effect that significantly boosted methane yield in the photocatalytic process. As a result, the ZnO/CuO/Ti<sub>3</sub>C<sub>2</sub> NSs/ILs heterojunction nanocomposite demonstrated significantly enhanced photocatalytic activity for dense-phase CO<sub>2</sub> reduction compared to pristine ZnO nanoparticles. Using water as a hydrogen source, ZnO/0.5CuO/Ti<sub>3</sub>C<sub>2</sub> NSs exhibit a very high total yield for liquid CO<sub>2</sub> reduction (62 bar and 22 °C), reaching 136.9 mmol h⁻¹ g⁻¹ for CO and 30.2 mmol h⁻¹ g⁻¹ for CH₄ under irradiation of a Xe arc lamp. This remarkable production rate marks a significant step forward in the development of efficient CO<sub>2</sub> reduction systems and presents a promising strategy for advancing solar-driven carbon conversion technologies.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"103 ","pages":"Article 103300"},"PeriodicalIF":8.4,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145797957","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
Solar photothermo-catalytic CO2 conversion into methane: Effect of phyllosilicates on the performance of Ni-Zn-Al layered double hydroxide-derived catalysts 太阳能光热催化CO2转化为甲烷:层状硅酸盐对Ni-Zn-Al层状双氧水衍生催化剂性能的影响
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-16 DOI: 10.1016/j.jcou.2025.103302
Luca Calantropo , Eleonora La Greca , Leonarda Francesca Liotta , Giuliana Impellizzeri , Antonino Gulino , Angelo Ferlazzo , Libera Vitiello , Sabrina Carola Carroccio , Salvatore Scirè , Roberto Fiorenza
The development of efficient catalysts for CO₂ utilization is a key challenge for industrial sustainability. This study explores the photothermo-catalytic methanation of CO₂ using Ni-Zn-Al Layered Double Hydroxide-derived (LDHd) catalysts modified with phyllosilicates (Montmorillonite K30 and Halloysite). LDH precursors were synthesized by co-precipitation and hydrothermal treatment, then calcined and reduced leading to the formation of mixed oxides and metallic Ni and Zn nanoparticles. Catalytic performances were evaluated at 1 atm and 350 °C. The Ni-Zn-Al LDHd catalyst achieved high CO₂ conversion (86 %) and CH₄ selectivity (>99 %) under photothermo-catalytic conditions, outperforming commercial Ni systems. Incorporation of halloysite, thermally treated at 200 °C, further increased CO₂ conversion to 92 % with the same high CH₄ selectivity. This improved performance is attributed to enhanced surface area, optical absorption and moderate–strong basic sites from LDHd–Halloysite interaction. In contrast, Montmorillonite modification, despite cetyltrimethylammonium bromide (CTAB) intercalation, resulted in lower activity and selectivity, due to weaker basicity and ineffective LDHd interaction. The Ni-Zn-Al LDHd/halloysite catalyst exhibited excellent stability during 20 h of continuous photothermo-catalytic test at 350 °C. These results demonstrate the potential of phyllosilicate-modified LDH-derived catalysts, with low metals content, for efficient CO₂ methanation under solar irradiation.
开发高效的CO₂利用催化剂是工业可持续发展的关键挑战。利用层状硅酸盐(蒙脱土K30和高岭土)改性的Ni-Zn-Al层状双氢氧化物(LDHd)催化剂,研究了CO 2的光热催化甲烷化反应。通过共沉淀法和水热法合成LDH前驱体,煅烧还原得到混合氧化物和金属Ni、Zn纳米颗粒。在1 atm和350℃条件下评价催化性能。Ni- zn - al LDHd催化剂在光热催化条件下具有较高的CO₂转化率(86% %)和CH₄选择性(>99 %),优于商业Ni体系。加入高岭土,在200°C下进行热处理,进一步提高CO₂转化率至92 %,并具有相同的高CH₄选择性。这种性能的提高是由于ldh - halloyite相互作用增强了表面积、光吸收和中强碱性位点。相比之下,蒙脱土改性后,尽管插入十六烷基三甲基溴化铵(CTAB),但由于碱度较弱且LDHd相互作用无效,活性和选择性较低。在350℃的连续光热催化测试中,Ni-Zn-Al LDHd/高岭土催化剂在20 h内表现出优异的稳定性。这些结果表明,在太阳照射下,层状硅酸盐改性低金属含量的ldh衍生催化剂具有高效二氧化碳甲烷化的潜力。
{"title":"Solar photothermo-catalytic CO2 conversion into methane: Effect of phyllosilicates on the performance of Ni-Zn-Al layered double hydroxide-derived catalysts","authors":"Luca Calantropo ,&nbsp;Eleonora La Greca ,&nbsp;Leonarda Francesca Liotta ,&nbsp;Giuliana Impellizzeri ,&nbsp;Antonino Gulino ,&nbsp;Angelo Ferlazzo ,&nbsp;Libera Vitiello ,&nbsp;Sabrina Carola Carroccio ,&nbsp;Salvatore Scirè ,&nbsp;Roberto Fiorenza","doi":"10.1016/j.jcou.2025.103302","DOIUrl":"10.1016/j.jcou.2025.103302","url":null,"abstract":"<div><div>The development of efficient catalysts for CO₂ utilization is a key challenge for industrial sustainability. This study explores the photothermo-catalytic methanation of CO₂ using Ni-Zn-Al Layered Double Hydroxide-derived (LDHd) catalysts modified with phyllosilicates (Montmorillonite K30 and Halloysite). LDH precursors were synthesized by co-precipitation and hydrothermal treatment, then calcined and reduced leading to the formation of mixed oxides and metallic Ni and Zn nanoparticles. Catalytic performances were evaluated at 1 atm and 350 °C. The Ni-Zn-Al LDHd catalyst achieved high CO₂ conversion (86 %) and CH₄ selectivity (&gt;99 %) under photothermo-catalytic conditions, outperforming commercial Ni systems. Incorporation of halloysite, thermally treated at 200 °C, further increased CO₂ conversion to 92 % with the same high CH₄ selectivity. This improved performance is attributed to enhanced surface area, optical absorption and moderate–strong basic sites from LDHd–Halloysite interaction. In contrast, Montmorillonite modification, despite cetyltrimethylammonium bromide (CTAB) intercalation, resulted in lower activity and selectivity, due to weaker basicity and ineffective LDHd interaction. The Ni-Zn-Al LDHd/halloysite catalyst exhibited excellent stability during 20 h of continuous photothermo-catalytic test at 350 °C. These results demonstrate the potential of phyllosilicate-modified LDH-derived catalysts, with low metals content, for efficient CO₂ methanation under solar irradiation.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"103 ","pages":"Article 103302"},"PeriodicalIF":8.4,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145797953","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
Numerical simulation and optimization of a CO2 absorption tower using solution absorption method for capture 采用溶液吸收法捕集的CO2吸收塔的数值模拟与优化
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-13 DOI: 10.1016/j.jcou.2025.103303
Fengqiang Miao , Xinyu Wang , Hao Wan , Xiangming Zhao , Linyang Zhang , Feng Xu , Dongdong Ren , Jianxiang Guo
The solution absorption method is one of the commonly used approaches in Carbon Capture, Utilization, and Storage. The performance and operating parameters of the absorption tower significantly affect CO2 capture efficiency. This study investigated the impact of various input parameters and tower structure on carbon capture efficiency. Findings reveal that among variations in inlet temperatures for both gas and liquid phases, adjusting the absorbent liquid temperature markedly influences capture efficiency, while changes in flue gas inlet temperature have minimal impact. Observing gas-liquid velocity variations shows that reducing both velocities generally increases CO2 capture efficiency; however, for MEA solutions, further reduction below 0.5 m/s leads to decreased efficiency. Additionally, a 10 % CO2 concentration is more easily captured than higher concentrations. Research on packing layer structural characteristics indicates that porosity changes produce opposing effects, with an optimal porosity level of 36 %. Increasing tower height also enhances absorption capacity, with calculations identifying 7 m as the optimal height.
溶液吸收法是碳捕获、利用和封存中常用的方法之一。吸收塔的性能和运行参数对CO2捕集效率有显著影响。研究了不同输入参数和塔结构对碳捕集效率的影响。研究结果表明,在气相和液相入口温度的变化中,调节吸收液温度对捕集效率有显著影响,而烟气入口温度的变化对捕集效率的影响最小。观察气液速度变化表明,降低两种速度通常会提高CO2捕集效率;然而,对于MEA解决方案,进一步降低到0.5 m/s以下会导致效率下降。此外,10 %的二氧化碳浓度比更高的浓度更容易被捕获。对充填层结构特征的研究表明,孔隙度变化产生相反的效果,最佳孔隙度为36% %。增加塔的高度也提高了吸收能力,通过计算确定7 m为最佳高度。
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引用次数: 0
Advanced solar–geothermal polygeneration system for CO2-based power, hydrogen, and freshwater recovery via transcritical CO2 rankine cycle 先进的太阳能-地热多联产系统,通过跨临界二氧化碳朗肯循环用于二氧化碳发电、氢气和淡水回收
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-13 DOI: 10.1016/j.jcou.2025.103301
Yassine Bouazzi , Zakarya Ahmed , Saman Ahmad Aminian , Veyan A. Musa , Mohamed Shaban , Narinderjit Singh Sawaran Singh , Wajdi Rajhi , Borhen Louhichi
The use of carbon dioxide as a high-performance working-fluid in advanced thermodynamic cycles provides a compelling route for developing low-carbon, multi-output renewable-energy systems. The study develops and assesses an advanced hybrid solar–geothermal polygeneration facility designed to produce electricity, hydrogen, and freshwater under the real resource conditions of the Harrat Rahat geothermal zone in Saudi Arabia. The configuration combines a double-flash geothermal cycle with a Transcritical CO2 Rankine cycle, a Kalina cycle, an alkaline electrolyser, and a reverse-osmosis desalination unit, supported by parabolic trough solar thermal augmentation. A full 3E+S evaluation—covering energy, exergy, economic, and sustainability metrics—is carried out alongside multi-objective optimization using the Secretary Bird metaheuristic algorithm. Under the real resource inputs of the Harrat Rahat site—geothermal reservoir temperatures exceeding 220 °C and mean solar irradiance of ∼6.6 kWh m−2 day−1, the results show the system could deliver 3.65 MW of net electricity, 9.35 kg.h−1 of hydrogen, and 10.23 m3.h−1 of freshwater, with overall energy and exergy efficiencies of 42.7 % and 38.18 %. Optimization enhances exergy efficiency by about 1.54 % and lowers the levelized cost of energy by roughly 2.2 %, yielding an LCOE of 0.04039 USD/MJ and a sustainability index of 0.238. Exergy-destruction profiling shows that condensers (≈47 %) and the solar thermal subsystem (≈16 %) are the main contributors to irreversibility. Overall, the results indicate that integrating high-enthalpy geothermal resources with concentrated solar power and advanced thermodynamic cycles can deliver a robust, efficient, and economically competitive polygeneration pathway suited to arid regions with strong energy and water needs.
在先进的热力学循环中,二氧化碳作为高性能工作流体的使用为开发低碳、多输出的可再生能源系统提供了一条引人注目的途径。该研究开发并评估了一种先进的混合太阳能-地热多联产设施,该设施旨在在沙特阿拉伯Harrat Rahat地热带的实际资源条件下生产电力、氢气和淡水。该结构结合了双闪蒸地热循环、跨临界CO2朗肯循环、Kalina循环、碱性电解槽和反渗透海水淡化装置,并由抛物面槽太阳能热增强装置提供支持。一个完整的3E+S评估——包括能源、能源、经济和可持续性指标——与多目标优化一起使用秘书鸟元启发式算法进行。在哈拉特拉哈特地热储层温度超过220°C,平均太阳辐照度为~ 6.6 kWh m−2 day−1的实际资源投入下,结果表明,该系统可提供3.65 MW净电力,9.35 kg.h−1氢气和10.23 m3.h−1淡水,总能量和火用效率分别为42.7% %和38.18 %。优化后的火用效率提高了约1.54 %,平准化能源成本降低了约2.2 %,LCOE为0.04039美元/焦耳,可持续性指数为0.238。火能破坏分析表明,冷凝器(≈47 %)和太阳热子系统(≈16 %)是不可逆性的主要贡献者。总体而言,研究结果表明,将高焓地热资源与聚光太阳能和先进的热力学循环相结合,可以提供一个强大的、高效的、具有经济竞争力的多联产途径,适用于能源和水需求旺盛的干旱地区。
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引用次数: 0
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Journal of CO2 Utilization
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