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Ti(OH)4-assisted amine-modified silica aerogels for enhancing CO2 adsorption capacity and amine efficiency Ti(OH)4辅助胺修饰二氧化硅气凝胶提高CO2吸附能力和胺效率
Pub Date : 2025-12-31 DOI: 10.1016/j.ccst.2025.100566
Jin Young Joo , Monica Louise T. Triviño , Hyung-Ho Park , Jeong Gil Seo
Amine-modified silica aerogels are promising CO2 sorbents owing to their high surface area, tunable pore structure, and strong chemisorption interactions between CO2 and amine groups. However, their amine efficiency and adsorption capacity remain limited for practical applications. In this study, Ti(OH)4 was introduced as an additive to enhance both the structural and functional performance of amine-grafted silica aerogels. The incorporation of Ti(OH)4 modified the pore structure, improved the dispersion of amine groups within the silica network, and increased the number of available hydroxyl groups. As a result, the Ti(OH)4-containing samples exhibited improved CO2 capture performance and higher amine efficiency under both dry and humid conditions. Detailed analyses further reveal that the additive promoted the formation of bicarbonate intermediates in humid environments, leading to a significant enhancement in adsorption performance. This was supported by TPD-MS results, which showed an increased ratio of desorbed H2O to CO2, indicating that Ti(OH)4 actively participated in the cooperative reaction between CO2, H2O, and amine species. The additive-containing sample achieved amine efficiencies of up to 0.475 mol-CO2/mol-N under dry conditions and 0.905 mol-CO2/mol-N under humid conditions, which is substantially higher than that of the additive-free sample. These findings demonstrate that Ti(OH)4 serves as an effective multifunctional additive that enhances amine dispersion and improves CO2-amine interactions, providing a suitable strategy for developing high-performing amine-based CO2 adsorbents for practical applications.
胺改性二氧化硅气凝胶由于其高表面积、可调节的孔隙结构以及二氧化碳与胺基之间强的化学吸附作用而成为很有前途的二氧化碳吸附剂。然而,它们的胺效率和吸附能力在实际应用中仍然有限。在本研究中,Ti(OH)4作为添加剂被引入以提高胺接枝二氧化硅气凝胶的结构和功能性能。Ti(OH)4的掺入改变了孔结构,改善了胺基在二氧化硅网络中的分散,增加了可用羟基的数量。结果表明,含Ti(OH)4的样品在干燥和潮湿条件下均表现出更好的CO2捕获性能和更高的胺效率。进一步的详细分析表明,添加剂促进了潮湿环境中碳酸氢盐中间体的形成,从而显著提高了吸附性能。TPD-MS结果也支持了这一观点,结果显示解吸H2O与CO2的比例增加,表明Ti(OH)4积极参与了CO2、H2O和胺类之间的协同反应。在干燥条件下,含添加剂样品的胺效率高达0.475 mol-CO2/mol-N,在潮湿条件下为0.905 mol-CO2/mol-N,大大高于无添加剂样品。这些研究结果表明,Ti(OH)4是一种有效的多功能添加剂,可以增强胺的分散性,改善二氧化碳与胺的相互作用,为开发具有实际应用价值的高性能胺基二氧化碳吸附剂提供了合适的策略。
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引用次数: 0
Zeolitic imidazolate framework/graphene hybrid nanocomposites for downhole CO2/H2 separation during in-situ hydrogen production from hydrocarbon reservoirs 沸石咪唑盐框架/石墨烯杂化纳米复合材料用于油藏现场制氢过程中的井下CO2/H2分离
Pub Date : 2025-12-31 DOI: 10.1016/j.ccst.2025.100565
Bennet Nii Tackie-Otoo , Mobeen Murtaza , Mahmoud Abdelnaby , Sagheer A. Onaiz , Shirish Patil , Muhammad Shahzad Kamal , Mohamed Mahmoud , Arshad Raza , Amro Elsayed
Selective CO2 separation from H₂-rich streams is crucial for advancing in-situ hydrogen production from depleted natural gas reservoirs. This study investigates pristine-graphene-based nanocomposites of ZIF-8 and ZIF-67 as solid sorbents for high-pressure CO2/H2 separation. Graphene@ZIF-8 and Graphene@ZIF-67 were synthesized via a modified sonochemical route that enabled uniform ZIF crystal growth on graphene. XRD confirmed complete retention of the sodalite topology with no impurity phases. SEM and BET analyses showed that incorporating graphene increased the BET surface area of ZIF-8 from 1284 to 1471 m2/g (+15%) and ZIF-67 from 1116 to 1413 m2/g (+27%), while also increasing total pore volume by ∼10-16%. CO2 adsorption improved substantially, with Graphene@ZIF-8 (75 cm3/g) and Graphene@ZIF-67 (65 cm3/g) exhibiting ∼2× higher uptake than their pristine ZIF counterparts (38 and 25 cm3/g, respectively). Langmuir monolayer capacities similarly increased from 105 to 404 cm3 (+285%) for ZIF-8 and from 48 to 354 cm3 (+637%) for ZIF-67 upon graphene hybridization. In contrast, H2 uptake remained lower than CO2, producing enhanced CO2/H2 selectivity; Graphene@ZIF-8 achieved a maximum selectivity of ∼11, compared to ∼10 for ZIF-8 and <4 for ZIF-67. These improvements demonstrate that pristine-graphene-supported ZIF nanocomposites provide significantly enhanced adsorption capacity and selectivity, making them strong candidates for CO2 capture from H2-rich gas streams in subsurface hydrogen production.
从富H 2流中选择性分离CO2对于推进枯竭天然气储层的原位制氢至关重要。本研究研究了ZIF-8和ZIF-67纳米复合材料作为高压CO2/H2分离的固体吸附剂。通过改进的声化学方法合成了Graphene@ZIF-8和Graphene@ZIF-67,使ZIF晶体在石墨烯上均匀生长。x射线衍射证实完全保留了钠石的拓扑结构,没有杂质相。SEM和BET分析表明,石墨烯的掺入使ZIF-8的BET表面积从1284增加到1471 m2/g(+15%),使ZIF-67的BET表面积从1116增加到1413 m2/g(+27%),同时也使总孔隙体积增加了10-16%。二氧化碳吸收量显著提高,Graphene@ZIF-8 (75 cm3/g)和Graphene@ZIF-67 (65 cm3/g)的吸收量比原始ZIF对应物(分别为38和25 cm3/g)高2倍。石墨烯杂交后,ZIF-8的Langmuir单层容量从105增加到404 cm3 (+285%), ZIF-67的Langmuir单层容量从48增加到354 cm3(+637%)。相比之下,H2吸收量仍然低于CO2吸收量,从而提高了CO2/H2的选择性;Graphene@ZIF-8的最大选择性为~ 11,而ZIF-8的最大选择性为~ 10,ZIF-67的最大选择性为<;4。这些改进表明,原始石墨烯负载的ZIF纳米复合材料具有显著增强的吸附能力和选择性,使其成为地下氢气生产中富h2气流中CO2捕获的强有力候选材料。
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引用次数: 0
Impact of uncertainty in Utsira formation temperature and salinity on CO2 storage: A field-scale reactive transport simulation study Utsira地层温度和盐度的不确定性对CO2储存的影响:现场尺度反应输运模拟研究
Pub Date : 2025-12-31 DOI: 10.1016/j.ccst.2025.100567
Mohamed Gamal Rezk , Ahmed Farid Ibrahim
Saline aquifers offer large storage capacities for carbon dioxide (CO2) geo-sequestration. However, key parameters such as aquifer temperature and brine salinity often remain uncertain, especially in thick formations. These uncertainties can significantly influence the CO2 reactive transport and trapping. Hence, this study aims to quantify the impact of such uncertainties on CO2 hydrodynamics and geochemical interactions, utilizing field-scale data of the Sleipner CO2 storage project, where temperature and salinity are treated as uncertain parameters. A response surface methodology (RSM) was employed to systematically investigate these uncertainties and quantify their impact on CO2 trapping. To do so, a three-dimensional reactive transport model was constructed to simulate multiphase flow, mineral dissolution and precipitation, and CO2 trapping mechanisms. The geological model of the Utsira formation was modified to match the plume dynamics. Formation temperatures ranging from 35 °C to 41 °C and salinities between 0.5 and 2 times that of seawater (33,500 ppm) were tested. Geochemical reactions were modeled using equilibrium and kinetic approaches, with temperature-dependent parameters governing the mineral changes. Proxy models generated with the RSM framework were used to quantify probabilistic uncertainty in the four CO2 trapping mechanisms. The simulation results showed that CO2 trapping mechanisms were sensitive to the uncertainty in aquifer temperature and salinity over 300 years. The highest temperature case exhibited the lowest capillary-trapped and solubility-trapped CO2. While both mechanisms increased at lower aquifer temperatures. The temperature also had a significant impact on both the onset time of CO2 mineralization and the total mineral trapping. Lower brine salinity improved dissolution trapping (from 42 % at 2S to 50.4 % at 0.5S), but mineralization varied minimally with salinity. The brine density contrast in the lower-salinity cases improved convective mixing, promoting CO2 dissolution. The uncertainty analysis further revealed distinct probabilistic ranges for each trapping mechanism, highlighting the dominant influence of salinity on physical trapping processes and temperature on mineral trapping.
含盐含水层为二氧化碳的地质封存提供了巨大的储存能力。然而,含水层温度和盐水盐度等关键参数通常仍然不确定,特别是在厚地层中。这些不确定性会显著影响CO2的反应性输运和捕集。因此,本研究旨在利用Sleipner CO2封存项目的现场尺度数据,将温度和盐度作为不确定参数,量化这些不确定性对CO2流体动力学和地球化学相互作用的影响。采用响应面法(RSM)系统地研究了这些不确定性,并量化了它们对CO2捕集的影响。为此,构建了三维反应输运模型,模拟了多相流、矿物溶解和沉淀以及CO2捕集机制。对Utsira地层的地质模型进行了修改,以匹配羽流动力学。测试的地层温度范围为35℃~ 41℃,盐度为海水的0.5 ~ 2倍(33,500 ppm)。地球化学反应使用平衡和动力学方法建模,与温度相关的参数控制矿物变化。利用RSM框架生成的代理模型对四种CO2捕集机制的概率不确定性进行了量化。模拟结果表明,CO2捕集机制对300多年来含水层温度和盐度的不确定性非常敏感。在温度最高的情况下,毛细管捕获和溶解度捕获的CO2含量最低。而这两种机制在含水层温度较低时都有所增加。温度对CO2矿化开始时间和总矿物圈闭均有显著影响。较低的盐水盐度改善了溶解捕获(从2S时的42%提高到0.5S时的50.4%),但矿化随盐度变化最小。低盐度条件下的盐水密度对比改善了对流混合,促进了CO2的溶解。不确定性分析进一步揭示了每种捕获机制的不同概率范围,突出了盐度对物理捕获过程的主导影响和温度对矿物捕获的主导影响。
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引用次数: 0
Energy-optimised cryogenic CO2 capture for cement production decarbonisation: process design and techno-economic analysis 能源优化的水泥生产脱碳低温CO2捕集:工艺设计和技术经济分析
Pub Date : 2025-12-27 DOI: 10.1016/j.ccst.2025.100563
Leonardo Varnier , Federico d’Amore , Bart de Groot , Fabrizio Bezzo
Achieving net-zero emissions in the cement sector requires the development of effective carbon capture technologies to address process-related emissions from limestone calcination. While much of the current research and applications focus on more conventional methods such as chemical absorption and oxyfuel, cryogenic CO2 capture offers potential advantages in energy efficiency, capture rate, and product purity, though it remains underexplored at an industrial scale.
This study presents a comprehensive assessment of cryogenic CO2 capture for cement applications in the EU, including thermodynamic modelling, process design and optimisation, and techno-economic analysis. Two process configurations targeting 90% and 95% capture at 99.9%mass CO2 purity are benchmarked. The 90% capture design achieves an energy penalty of 1.19 MJel/kgCO2, corresponding to a threefold increase in electricity consumption compared to an unabated cement plant. Sensitivity analysis demonstrates consistent energy performance across a 17-28%mol range of flue gas compositions. Increasing the capture rate from 90% to 95% maintains the energy penalty nearly constant (1.19-1.21 MJel/kgCO2), with only marginal economic impact. At 95% capture, the incremental cost of clinker production rises by 5% compared to 90% capture, while the higher CO2 avoidance yields a similar cost of avoided CO2 (127-128 €/tCO2).
From an economic perspective, cryogenic capture significantly outperforms conventional MEA-based capture, while remaining slightly less competitive than oxyfuel and calcium looping under current EU energy mix conditions. Overall, cryogenic capture emerges as an energy-efficient and economically viable post-combustion option for cement industry decarbonisation, with the added benefit of delivering a high-purity CO2 stream suitable for storage or utilisation.
实现水泥行业的净零排放需要开发有效的碳捕获技术,以解决石灰石煅烧过程中的相关排放问题。虽然目前大部分研究和应用都集中在更传统的方法上,如化学吸收和含氧燃料,但低温二氧化碳捕集在能源效率、捕集率和产品纯度方面具有潜在的优势,尽管在工业规模上仍未得到充分的探索。本研究对欧盟水泥低温二氧化碳捕集的应用进行了全面评估,包括热力学建模、工艺设计和优化以及技术经济分析。以99.9%的二氧化碳质量纯度为基准,对两种工艺配置进行了90%和95%的捕集。90%的捕集设计实现了1.19 MJel/kgCO2的能量损失,与未减排量的水泥厂相比,相当于电力消耗增加了三倍。灵敏度分析表明,在17-28%mol的烟气成分范围内,能量表现是一致的。将捕集率从90%提高到95%,能量损失几乎保持不变(1.19-1.21 MJel/kgCO2),只有边际经济影响。在95%的捕集率下,与90%的捕集率相比,熟料生产的增量成本增加了5%,而更高的二氧化碳避免率产生了相似的二氧化碳避免成本(127-128欧元/吨二氧化碳)。从经济角度来看,低温捕集明显优于传统的基于mea的捕集,但在当前欧盟能源结构条件下,其竞争力略低于氧燃料和钙环。总的来说,低温捕集是水泥行业脱碳的一种节能且经济可行的燃烧后选择,其额外的好处是提供适合储存或利用的高纯度二氧化碳流。
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引用次数: 0
Hybrid monitoring framework for geological CO2 storage: Comparative insights from nuclear magnetic resonance (NMR) and conventional techniques 地质二氧化碳储存的混合监测框架:来自核磁共振(NMR)和传统技术的比较见解
Pub Date : 2025-12-25 DOI: 10.1016/j.ccst.2025.100561
Zahrah Ghannam , Mazin Osman , Omer Mohamed Bakri , Mohamed Mahmoud , Muhammad Shahzad Kamal , Rahul Gajbhiye , Ahmed Abdulhamid Mahmoud
Effective tracking of the geological carbon dioxide (CO2) storage is very important in ensuring the safety of the environment and adherence to storage rules. This review discusses the classic geophysical techniques such as 4D seismic, electromagnetic (EM), and gravimetry and their abilities are compared to nuclear magnetic resonance (NMR), which is an emerging technology that improves monitoring on a microscopic scale. Conventional methods are appropriate to map the movement of plumes and structural variations but are not good enough to see important processes such as residual trapping, changes in wettability, and fluid dynamics at the pore-scale. Conversely, NMR quantitatively describes fluid interactions and phase behavior at the pore level and is able to give quantitative information on CO2 saturation and trapping processes.
This review shed light on how NMR, under a combination with conventional geophysical methods, can form a hybrid monitoring system that can offer the pore-scale accuracy of the monitoring approach, and the field-scale extent of the monitoring framework. Through machine learning, built-in workflows now can combine seismic, pressure, and fluid chemistry data increasing predictive accuracy and uncertainty quantification. This hybrid monitoring method will greatly enhance the credibility of the CO2 storage measurements through the real-time identification of the possible leakage and the reservoir maintenance. Future CO2 storage projects can realize this by placing NMR in greater monitoring networks.
有效的地质二氧化碳封存跟踪对确保环境安全、遵守封存规则具有十分重要的意义。本文讨论了经典的地球物理技术,如四维地震、电磁(EM)和重力测量,并将它们的能力与核磁共振(NMR)进行了比较,核磁共振是一种新兴的技术,可以改善微观尺度的监测。传统的方法适合于绘制羽流的运动和结构变化,但不足以在孔隙尺度上观察残余捕获、润湿性变化和流体动力学等重要过程。相反,核磁共振定量描述流体相互作用和孔隙水平的相行为,并能够提供二氧化碳饱和度和捕获过程的定量信息。这篇综述揭示了核磁共振如何与传统的地球物理方法相结合,形成一个混合监测系统,可以提供监测方法的孔隙尺度精度和监测框架的现场尺度范围。通过机器学习,内置工作流程现在可以结合地震、压力和流体化学数据,提高预测准确性和不确定性量化。这种混合监测方法通过实时识别可能的泄漏和对储层的维护,大大提高了CO2储存测量的可信度。未来的二氧化碳储存项目可以通过将核磁共振放置在更大的监测网络中来实现这一点。
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引用次数: 0
Techno-economic and environmental optimization of structured-packing absorbers for amine-based post-combustion CO2 capture 胺基燃烧后CO2捕集结构填料的技术经济和环境优化
Pub Date : 2025-12-25 DOI: 10.1016/j.ccst.2025.100560
Md Sakib Hossain, Richard Barker, Timothy Cockerill, Harvey Thompson
Post combustion carbon capture and storage (CCS) using amine solvents is a mature and retrofittable technology where CO2 absorber design remains a critical determinant of cost, energy demand, and environmental footprint. Conventional studies typically size absorbers within proprietary simulators or apply simplified surrogates that limit transparency while excluding case specific design and material related impacts. This work develops a physics based, multi-objective optimization framework for structured-packing amine-based CCS absorbers in natural gas combined cycle (NGCC) plants that balances equilibrium driven mass transfer, hydraulics, techno-economic assessment, and cradle-to-gate embodied global warming potential (GWP) considerations. Several commercially available structured packings are evaluated and vendor relevant absorber geometries, which are height, diameter, packing type, and volume are directly linked to costs, reboiler duty, capture efficiency, and embodied emissions. Baseline optimization for a 250 MWe NGCC plant identifies knee-point optimum absorber designs achieving 95–97% capture at 40–52 million USD, 3.2–4.6 MJ/kmolsolvent reboiler duty, and 1300–1900 t CO2e embodied GWP. Sensitivity analyses show that plant scaling fundamentally alters packing selection, preferring high surface area packings (Montz BSH-400) for 100 MWe NGCC case. Meanwhile, at 750 MWe, hydraulically open packings (Montz B1–250) dominate optimum solutions to limit flooding and column parallelization. Steel emissions intensity further alters optimization outcomes with recycled steel reducing embodied emissions by up to 70%. Overall, the study establishes CCS absorber design as a scale-sensitive, multi-objective problem, and shows that design choices have significant implications for material use, embodied emissions, and overall system sustainability. The findings highlight the need to integrate environmental performance alongside cost and capture efficiency in CCS decision-making for large-scale and sustainable deployment.
使用胺类溶剂的燃烧后碳捕集与封存(CCS)是一项成熟的可改造技术,其中二氧化碳吸收器的设计仍然是成本、能源需求和环境足迹的关键决定因素。传统的研究通常在专有的模拟器中确定吸收剂的大小,或者采用简化的替代品,这限制了透明度,同时排除了具体的设计和材料相关的影响。这项工作为天然气联合循环(NGCC)工厂的结构填料胺基CCS吸收器开发了一个基于物理的多目标优化框架,该框架可以平衡平衡驱动的传质、水力学、技术经济评估和从摇篮到大门的全球变暖潜能值(GWP)考虑因素。我们评估了几种市售的结构化填料和供应商相关的吸收器几何形状,包括高度、直径、填料类型和体积,这些都与成本、再锅炉负荷、捕获效率和排放直接相关。250mwe NGCC电厂的基线优化确定了膝点最佳吸收器设计,在4000 - 5200万美元、3.2-4.6 MJ/ kmolmolsolvent re沸器负荷和1300-1900 t CO2e隐含的GWP下,实现了95-97%的捕集。敏感性分析表明,工厂规模从根本上改变了填料选择,对于100兆瓦的NGCC情况,更倾向于高表面积填料(Montz BSH-400)。同时,在750mwe时,水力开孔填料(Montz B1-250)是限制注水和柱间平行化的最佳解决方案。钢铁排放强度进一步改变了优化结果,回收的钢铁减少了高达70%的隐含排放量。总体而言,该研究将CCS吸收器设计确立为一个规模敏感、多目标的问题,并表明设计选择对材料使用、隐含排放和整体系统可持续性具有重要影响。研究结果强调了在大规模和可持续部署的CCS决策中,需要将环境绩效与成本和捕获效率结合起来。
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引用次数: 0
Diffusion explorer for the COF space: Data-driven discovery of high-performing COF membranes for gas separations COF空间的扩散探索者:数据驱动的高性能气体分离COF膜的发现
Pub Date : 2025-12-24 DOI: 10.1016/j.ccst.2025.100559
Gokhan Onder Aksu, Seda Keskin
Covalent organic frameworks (COFs) have recently emerged as highly promising candidates for membrane-based gas separations, exhibiting superior performance relative to conventional membrane materials. Nevertheless, the rapidly expanding number of COFs renders the experimental evaluation of each material’s membrane performance infeasible. In this study, we investigated the COF space comprising approximately 70,000 synthesized and hypothetical materials using high-throughput molecular dynamics (MD) simulations and machine learning (ML) for computing the diffusivities of CO2, CH4, H2, N2, and O2 gases. We generated an online toolbox by integrating our ML models to estimate gas diffusivities of any given COF material in seconds. Using the ML-predicted diffusivities, gas permeabilities and selectivities of COF membranes were assessed for seven industrially relevant separations; CO2/CH4, CO2/N2, H2/CO2, H2/N2, H2/CH4, O2/N2, N2/CH4. The performance of COF membranes was compared to traditional membrane materials, and the most promising COFs were identified and analyzed using molecular fingerprinting to reveal the critical structural and chemical features for accelerating the design of next-generation COF membranes.
共价有机框架(COFs)最近成为膜基气体分离的极有前途的候选者,相对于传统的膜材料具有优越的性能。然而,COFs数量的迅速增加使得对每种材料的膜性能进行实验评估变得不可行。在这项研究中,我们使用高通量分子动力学(MD)模拟和机器学习(ML)来计算CO2, CH4, H2, N2和O2气体的扩散系数,研究了由大约70,000种合成和假设材料组成的COF空间。我们通过集成我们的ML模型生成了一个在线工具箱,可以在几秒钟内估计任何给定COF材料的气体扩散率。利用机器学习预测的扩散系数,对7个工业相关分离的COF膜的气体渗透性和选择性进行了评估;Co2 / ch4 Co2 / n2 h2 / Co2 h2 / n2 h2 / n2 h2 / ch4 o2 / n2 n2 / ch4。将COF膜的性能与传统膜材料进行了比较,并利用分子指纹技术对最有前途的COF膜进行了鉴定和分析,揭示了COF膜的关键结构和化学特征,从而加快了下一代COF膜的设计。
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引用次数: 0
Engineering concrete as a carbon sink for sustainable infrastructure 工程混凝土作为可持续基础设施的碳汇
Pub Date : 2025-12-16 DOI: 10.1016/j.ccst.2025.100558
Chaolin Fang , Varenyam Achal
Concrete offers a unique opportunity to function as a scalable carbon sink by integrating physicochemical, mechanochemical, microbial, and magnesium-based pathways of CO₂ sequestration. This review synthesizes recent advances ranging from accelerated carbonation curing and pre-carbonated supplementary materials to bio-mediated mineralization and MgO-derived binders. Emerging applications—including 3D printing and biochar-enhanced aggregates—demonstrate measurable CO₂ uptake alongside mechanical and durability benefits. Life-cycle assessments consistently indicate 10–50% reductions in global-warming potential, yet challenges remain in scaling, energy demand, and long-term stability. Distinct from earlier reviews, this work unites mechanistic insights with industrial case studies and technoeconomic analysis to provide a roadmap for deploying carbon-sequestering concretes at scale. By coupling materials science, biotechnology, and digital monitoring with supportive policy frameworks, concrete can evolve from a major emitter into a durable carbon sink within circular-economy construction.
Tweetable abstract: This review shows how physicochemical, mechanochemical, biological and Mg-based pathways can turn concrete from a major CO₂ source into a durable, scalable carbon sink.
混凝土提供了一个独特的机会,通过整合物理化学、机械化学、微生物和镁基二氧化碳封存途径,作为一个可扩展的碳汇。本文综述了从加速碳化固化和预碳化补充材料到生物介导矿化和氧化镁衍生粘合剂的最新进展。新兴应用——包括3D打印和生物炭增强骨料——显示出可测量的二氧化碳吸收以及机械和耐用性方面的优势。生命周期评估一致表明,全球变暖潜力降低了10-50%,但在规模、能源需求和长期稳定性方面仍存在挑战。与之前的评论不同,这项工作将机械见解与工业案例研究和技术经济分析结合起来,为大规模部署碳封存混凝土提供了路线图。通过将材料科学、生物技术和数字监测与支持性政策框架相结合,混凝土可以从一个主要的排放源演变为循环经济建设中的持久碳汇。摘要:这篇综述展示了物理化学、机械化学、生物和镁基途径如何将混凝土从一个主要的二氧化碳源转变为一个持久的、可扩展的碳汇。
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引用次数: 0
Carbonation behavior of reactivated recycled concrete fines containing residual sand: Effects of Ca/Si ratio adjustment and activation temperature 含残砂再生混凝土细粒的碳化行为:钙硅比调节和活化温度的影响
Pub Date : 2025-12-15 DOI: 10.1016/j.ccst.2025.100557
Yutong Ju , Ye Li , Xiangping Xian , Tiejun Liu
The valorization of recycled concrete fines (RCF) into reactive binders offers a sustainable solution for mitigating construction waste and carbon emissions. However, embedded sand particles hinder phase development during thermal activation. This study explores thermally activated sand-containing RCF by adjusting calcium-to-silicon ratio via limestone addition to produce reactivated cementitious materials (RCM). Carbonation-cured RCMs were analyzed for phase evolution, microstructure, and strength. Results showed that higher activation temperature with Ca addition enhanced sand reactivity and mineral formation, transitioning from α′H-C2S and β-C2S below 1000 °C to low-reactivity CS or C3S2 at 1200 °C. Carbonation curing of RCM activated at 1000 °C with 20 wt.% limestone addition yielded the highest mechanical performance by optimizing phase reactivity, carbonation efficiency, and pore refinement, while lower strengths in other groups stemmed from insufficient CaCO3 and silica gel. Life cycle assessment showed a 61 % CO2 reduction compared to Portland cement, which validates thermochemical tuning for closed-loop RCF recycling.
将再生混凝土细粒(RCF)转化为活性粘合剂,为减少建筑垃圾和碳排放提供了可持续的解决方案。然而,在热活化过程中,嵌入的砂粒阻碍了相的发育。本研究通过添加石灰石来调节钙硅比,从而产生再活化胶凝材料(RCM),从而探索热活化含砂RCF。对碳化固化rcm进行了相演化、显微组织和强度分析。结果表明,Ca的加入提高了活化温度,增强了砂的反应性和矿物形成,从1000℃以下的α′H-C2S和β-C2S转变为1200℃时的低反应性CS或C3S2。在1000°C下,添加20 wt.%石灰石活化的RCM碳化固化通过优化相反应性、碳化效率和孔隙细化获得了最高的力学性能,而其他组的强度较低是由于CaCO3和硅胶不足。生命周期评估显示,与波特兰水泥相比,其二氧化碳排放量减少了61%,这证实了热化学调整可用于闭环RCF回收。
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引用次数: 0
Graphite–Ni synergy unlocks a hydrogen-free pathway for carbon based integrated CO₂ capture and utilisation (ICCU) 石墨-镍协同作用为碳基集成二氧化碳捕获和利用(ICCU)开辟了无氢途径
Pub Date : 2025-12-01 DOI: 10.1016/j.ccst.2025.100546
Junhan Lu, Xiaotong Zhao, Jia Hu, Bo Zong, Yuanyuan Wang, Chunfei Wu
Integrated carbon capture and utilisation (ICCU) is a promising technology to mitigate the impact of carbon emissions, as it combines sorbent regeneration and CO2 utilisation. ICCU has been intensively studied for reverse water shift reaction (RWGS), methanation and dry methane reforming (DRM). However, ICCU-RWGS and ICCU-Methanation rely on hydrogen, which compromises economic viability and safety, and the complex synthesis of DFMs for ICCU-DRM, requiring promoters or multilayer structures. To enhance the practicality of ICCU technology, here we investigated carbon-based ICCU (C-ICCU), which utilises the reverse Boudouard reaction with carbon as the reducing agent. In this study, we explored the key operational factors influencing C-ICCU performance, specifically Ni loading, the Ni/graphite mass, and temperature. Our findings indicate that Ni/graphite is a highly effective catalyst for the in-situ conversion of CO2 to CO. Specifically, a Ni loading of 3 wt.% or higher achieved a CO2 conversion greater than 95% at 650°C. Furthermore, in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis revealed the synergistic interactions between graphite and nickel. Specifically, graphite promotes CO2 generation while nickel catalyses its subsequent conversion. Our research demonstrates that the C-ICCU mechanism is a complex synergistic process involving the dynamic evolution of surface species. This work offers a promising, safer, and potentially more economical pathway for industrial carbon capture and utilisation.
综合碳捕获与利用(ICCU)是一种很有前途的技术,可以减轻碳排放的影响,因为它结合了吸附剂再生和二氧化碳利用。ICCU在逆水变换反应(RWGS)、甲烷化和干甲烷重整(DRM)中得到了广泛的研究。然而,ICCU-RWGS和iccu -甲烷化依赖于氢,这损害了经济可行性和安全性,并且ICCU-DRM的dms合成复杂,需要启动子或多层结构。为了提高ICCU技术的实用性,我们研究了碳基ICCU (C-ICCU),它利用碳作为还原剂进行反向Boudouard反应。在这项研究中,我们探讨了影响C-ICCU性能的关键操作因素,特别是Ni负载,Ni/石墨质量和温度。我们的研究结果表明,Ni/石墨是一种非常有效的催化剂,可以将CO2原位转化为CO。具体来说,在650°C下,3 wt.%或更高的Ni负载可以实现95%以上的CO2转化率。此外,原位漫反射红外傅立叶变换光谱(DRIFTS)分析揭示了石墨和镍之间的协同作用。具体来说,石墨促进二氧化碳的产生,而镍则催化其随后的转化。我们的研究表明,C-ICCU机制是一个复杂的协同过程,涉及地表物种的动态进化。这项工作为工业碳捕获和利用提供了一条有前途、更安全、潜在更经济的途径。
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Carbon Capture Science & Technology
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