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Real-time measurement and reaction rate analysis of CO2 absorption in cementitious materials by gas pressure monitoring using a batch reactor 间歇式反应器气体压力监测对胶凝材料中CO2吸收的实时测量和反应速率分析
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-13 DOI: 10.1016/j.jcou.2025.103273
Katsuya Namiki , Vincentius Wilson , Misuzu Takase , Toshio Osawa , Suguru Noda
CO2-absorbing concrete is being actively researched toward carbon neutrality. Real-time measurement of CO2 absorption is essential to accurately assess the progress of the carbonation reaction, elucidate the carbonation mechanism through reaction rate analysis, and optimize the carbonation conditions. In this study, a batch reactor was developed for real-time measurement of CO2 absorption in cementitious materials. A reaction tube and a CO2 container were placed in a constant-temperature oven and connected using a valve to initiate the carbonation reaction. The amount and rate of CO2 absorption were measured by monitoring the gas pressure with a time resolution of minutes, after correcting for the influence of water evaporation on pressure. The γ-2CaO·SiO2 powder absorbed 103 gCO2/kgsolid of CO2, achieving 21 % of its theoretical capacity within 5 min. A comparison between the CO2 absorption values determined by gas pressure monitoring and destructive analysis of carbonated samples revealed that the ratio remained stable for different materials and carbonation conditions, with an average of 1.00 and a standard deviation of 0.07. Additionally, 93 % of the data points were in the range of 0.90–1.10, demonstrating high reliability of the proposed method. Therefore, this method is a rapid, simple, and reliable means of evaluating CO2 absorption for various materials and carbonation conditions. Furthermore, this method can be combined with sample analysis to better understand the carbonation mechanism in CO2-absorbing concrete and determine optimal carbonation conditions.
二氧化碳吸收混凝土正朝着碳中和方向积极研究。实时测量CO2吸收量对准确评价碳酸化反应的进展、通过反应速率分析阐明碳酸化机理、优化碳酸化条件具有重要意义。在本研究中,开发了一种间歇式反应器,用于实时测量胶凝材料中的CO2吸收。将反应管和CO2容器置于恒温烘箱中,用阀门连接,开始碳酸化反应。在校正了水蒸发对压力的影响后,通过监测气体压力来测量CO2的吸收量和吸收率,时间分辨率为分钟。γ-2CaO·SiO2粉体吸附103 gCO2/kgsolid,在5 min内达到理论吸附量的21. %。通过气体压力监测和碳酸化样品破坏分析测定的CO2吸收值对比发现,该比值在不同材料和碳酸化条件下保持稳定,平均值为1.00,标准差为0.07。此外,93 %的数据点在0.90-1.10的范围内,表明所提出的方法具有较高的可靠性。因此,该方法是一种快速、简便、可靠的评估各种材料和碳化条件下CO2吸收率的方法。此外,该方法可以与样品分析相结合,更好地了解二氧化碳吸收混凝土的碳化机理,并确定最佳碳化条件。
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引用次数: 0
Gas diffusion electrodes enable enhanced energy efficiency of electrochemical CO2 reduction in natural brine-inspired electrolytes 气体扩散电极能够提高天然盐水激发电解质中电化学CO2还原的能量效率
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-12 DOI: 10.1016/j.jcou.2025.103268
Aykut Kas , Paniz Izadi , Ida Dinges , Markus Stöckl , Falk Harnisch
A circular economy demands efficient conversion of carbon dioxide (CO2) into valuable chemicals including C1-compounds like formate as building blocks for chemical production. The electrochemical CO2 reduction reaction (eCO2RR) in aqueous solutions is a promising approach, being limited by low CO2 solubility that restricts reaction rates and energy efficiency. In this study, we systematically investigated eCO2RR to formate using gas diffusion electrodes (GDEs) in electrolyte solutions with moderate (3 % w/v), high (10 % w/v), and hypersaline (17 % w/v) NaCl concentrations, representing natural saline water bodies. Notably, the presence of NaCl did not affect eCO2RR performance showing stable formate production rates of 1.30 ± 0.13 mmol L−1 h−1 cm−2 at a current density of 50 mA cm−2 across all salinities. Coulombic efficiencies (CE) for formate were similar across salinities starting at 80–90 % at 30 min and decreasing to ∼70 % after 120 min. Despite an expected ∼50 % decrease in CO₂ solubility with increasing salinity, GDEs ensured efficient CO₂ supply, preventing major performance losses. High salt electrolytes improved performance mainly by increasing electrolytic conductivity; however, benefits may also originate from an alternative anodic reaction, namely the chlorine evolution reaction (CER) instead of the oxygen evolution reaction (OER). At 17 % w/v NaCl, cell voltage decreased by 50.0 % and energy efficiency improved by up to 194.6 % when compared to sodium phosphate buffer, assuming CER was dominant. These findings indicate that the selection of anodic reaction is decisively influencing the energy efficiency of the eCO₂RR in saline electrolytes. Thus, we suggest that saline or brackish water can be sourced as electrolyte solutions for eCO2RR, offering a path towards large-scale carbon capture and utilization.
循环经济需要将二氧化碳(CO2)有效地转化为有价值的化学物质,包括甲酸盐等c1化合物,作为化学生产的基石。水溶液中的电化学CO2还原反应(eCO2RR)是一种很有前途的方法,但由于CO2溶解度低,限制了反应速率和能量效率。在这项研究中,我们系统地研究了eCO2RR在中(3 % w/v)、高(10 % w/v)和高盐(17 % w/v) NaCl浓度的电解质溶液中形成的过程。值得注意的是,NaCl的存在不影响eCO2RR的性能,在所有盐度下,电流密度为50 mA cm−2时,eCO2RR的甲酸产率稳定在1.30 ± 0.13 mmol L−1 h−1 cm−2。不同盐度下,甲酸盐的库仑效率(CE)相似,30 min时为80-90 %,120 min后降至70 %。尽管随着盐度的增加,CO 2溶解度预计会下降~ 50% %,但GDEs确保了有效的CO 2供应,避免了重大的性能损失。高盐电解质主要通过提高电解导电性来改善性能;然而,好处也可能来自另一种阳极反应,即氯析出反应(CER)而不是氧析出反应(OER)。假设CER占主导地位,在17 % w/v NaCl条件下,与磷酸钠缓冲液相比,电池电压降低50.0 %,能量效率提高194.6 %。这些结果表明,阳极反应的选择对含盐电解质中eCO₂RR的能量效率有决定性的影响。因此,我们建议可以将盐水或微咸水作为eCO2RR的电解质溶液,为大规模碳捕获和利用提供途径。
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引用次数: 0
A novel blend membrane modified Pebax-1657 with high-loading styrene-acrylonitrile copolymer for CO₂ separation 一种新型高负载苯乙烯-丙烯腈共聚物改性Pebax-1657共混膜用于CO₂分离
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-08 DOI: 10.1016/j.jcou.2025.103271
Fatemeh Shiri Jafarzadeh , Mostafa Vatani , Ahmadreza Raisi
One of the critical industrial processes is the removal of CO₂ from flue gas to control greenhouse gas emissions, enrich natural gas, and recover landfill gas. In this study, dense polymer blend membranes composed of Pebax (polyether-block-amide) and SAN (styrene–acrylonitrile) were prepared across a wide concentration range (0–100 wt%), and the effect of SAN loading on the structural properties and gas separation performance of the membranes was investigated. The fabricated blend membranes were characterized using various techniques, including X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and differential scanning calorimetry (DSC). The highest selectivity for CO2/N2 (126.3) and CO2/CH4 (33.2) was obtained for the blend membranes containing 20 wt% and 40 wt% SAN, respectively at a temperature of 25 °C and feed pressure of 8 bar. Moreover, the highest CH₄/N₂ selectivity (6.1) was observed for the 85/15 Pebax/SAN blend membrane under the same conditions. The results from the gas separation tests indicate that increasing the operating pressure and compactness within the polymer matrix in the presence of high molecular weight SAN significantly improves gas selectivity. In this regard, the 80/20 Pebax/SAN membrane, with a CO₂ permeability of 37.9 Barrer and CO2/N2 selectivity of 126.3 at 8 bar, surpassed Robeson’s 2008 upper bound and approached the previous Robeson upper bound with a CO2/CH4 selectivity of 26.9.
关键的工业过程之一是从烟道气中去除CO 2以控制温室气体排放,富集天然气并回收垃圾填埋气。在本研究中,制备了由Pebax(聚醚-嵌段酰胺)和SAN(苯乙烯-丙烯腈)在较宽的浓度范围(0-100 wt%)内组成的致密聚合物共混膜,并研究了SAN负载对膜结构性能和气体分离性能的影响。利用x射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描电镜(SEM)和差示扫描量热法(DSC)等技术对制备的共混膜进行了表征。当温度为25℃,进料压力为8 bar时,含20 wt%和40 wt% SAN的共混膜对CO2/N2(126.3)和CO2/CH4(33.2)的选择性最高。在相同条件下,85/15 Pebax/SAN共混膜的CH₄/N₂选择性最高(6.1)。气体分离实验结果表明,在高分子量SAN存在的情况下,增加操作压力和聚合物基质内的致密度可以显著提高气体选择性。因此,80/20 Pebax/SAN膜在8 bar下的CO₂渗透率为37.9 Barrer, CO2/N2选择性为126.3,超过了Robeson的2008上限,并以26.9的CO2/CH4选择性接近之前的Robeson上限。
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引用次数: 0
From material characterization to process simulation: Performance evaluation of amine-infused resins for CO2 capture 从材料表征到过程模拟:用于CO2捕获的胺注入树脂的性能评估
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-07 DOI: 10.1016/j.jcou.2025.103272
Geonwoo Jeong , Jongyeon Jung , Woojin Go , Chelim Min , Zhijian Wan , Colin D. Wood , Yutaek Seo
Selective capture of CO2 using solid CO2 sorbents provides an effective solution for a simplified CO2 capture process, however it demands high CO2 capture performance with low regeneration energy. A solid adsorbent incorporating diethanolamine (DEA) within a cross-linked polystyrene based porous ion-exchange resin was synthesized. DEA was incorporated into the channels of the resin by infusion, denoted as an amine-infused resin (AIR). Performance of the AIR in CO2 adsorption was evaluated, then the desorption properties were measured along with the surface morphology and particle size distribution. The commercial process simulator Aspen Adsorption was employed to model the single-bed experimental system. Simulation results showed good agreement with experimental data, particularly in terms of breakthrough behavior and CO2 holdup during adsorption–desorption cycles. The validated model was used to design a CO2 capture system adopting temperature swing adsorption (TSA) for CO2 removal from gas stream. The five-column TSA unit operating at 2 bar produced a CO2 stream with three-step cycle of adsorption, desorption by hot water, and cooling. The overall energy consumption of 3.02 GJ/tCO2 was estimated from the total amount of heat during desorption of 53.9 kJ/mol CO2. The reduced regeneration temperature and energy requirements for the AIR results in improved productivity. The findings of this study highlight the potential of AIR as a promising alternative for CO2 capture process with several advantages, including comparable CO2 capture performance, efficient regeneration, and scalability.
利用固体CO2吸附剂选择性捕集CO2为简化CO2捕集过程提供了一种有效的解决方案,但它对CO2捕集性能要求高,再生能量低。在交联聚苯乙烯多孔离子交换树脂中合成了二乙醇胺(DEA)固体吸附剂。通过输注将DEA掺入树脂通道中,记为胺注入树脂(AIR)。考察了空气对CO2的吸附性能,并对其解吸性能、表面形貌和粒径分布进行了测定。利用商业过程模拟器对单床实验系统进行模拟。模拟结果与实验数据吻合较好,特别是在吸附-解吸循环过程中的突破行为和CO2含率方面。利用该模型设计了一套采用变温吸附法(TSA)去除气流中CO2的CO2捕集系统。在2 bar下工作的五柱TSA装置产生二氧化碳流,经过吸附、热水解吸和冷却的三步循环。由解吸过程的总热量53.9 kJ/mol CO2估算出总能耗为3.02 GJ/tCO2。空气再生温度和能量需求的降低提高了生产效率。这项研究的结果强调了空气作为一种有希望的二氧化碳捕获过程替代方案的潜力,它具有几个优势,包括可比的二氧化碳捕获性能、高效的再生和可扩展性。
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引用次数: 0
Tuning catalyst performance in methane dry reforming via microwave irradiation of Nickel-Silicon carbide systems 微波辐照镍-碳化硅体系对甲烷干重整催化剂性能的调整
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1016/j.jcou.2025.103270
Christel Olivier Lenge Mbuya , Kunal Pawar , Mitra Jafari , Parisa Shafiee , Chike George Okoye Chine , Pilar Tarifa , Bogdan Dorneanu , Harvey Arellano-Garcia
The dry reforming of methane (DRM) is a promising route for converting greenhouse gases such as methane (CH4) and carbon dioxide (CO2) into valuable syngas, hydrogen (H2) and carbon monoxide (CO). However, traditional nickel (Ni)-based catalysts suffer from rapid deactivation due to carbon deposition and sintering, especially when supported on low thermal conductivity materials. In this work, a novel post-synthesis microwave irradiation (MIR) treatment is introduced to systematically optimize the performance of Ni – β – SiC and Ni – Ti – Cβ – SiC catalysts for DRM. Unlike previous studies that have used MIR during reaction or with different supports, this approach tunes the metal – support interactions and textural properties of Ni – β – SiC and Ni – Ti – Cβ – SiC catalysts by varying the MIR exposure time after catalyst synthesis. MIR post-treatment (10–25 s) increased the CH4 conversion to 65 % and the CO2 conversions to 62 % for Ni–β–SiC catalysts and improved the H₂/CO ratio to 0.80, with stable performance over 20 h. For Ni–Ti–Cβ–SiC, MIR (10–20 s) maintained CH4 conversion up to 60 % and CO2 conversion to 58 % over 20 h, while the untreated catalyst, though initially higher, deactivated rapidly. Excessive MIR (30 s) reduced performance for both catalyst types, underscoring the need for optimal exposure time. These findings demonstrate post-synthesis MIR provides a tuneable approach for enhancing both the activity and durability of Ni/SiC – based DRM catalysts through controlled modification of metal – support interactions. This work offers new insights for the design of robust catalysts aimed at greenhouse gas utilization and sustainable syngas production, with activity and stability enhancements linked to controlled changes in metal – support interactions.
甲烷干重整(DRM)是将甲烷(CH4)和二氧化碳(CO2)等温室气体转化为有价值的合成气、氢气(H2)和一氧化碳(CO)的一种有前途的途径。然而,传统的镍基催化剂由于碳沉积和烧结而快速失活,特别是在低导热材料上支撑时。本文介绍了一种新的合成后微波辐照(MIR)处理方法,系统地优化了Ni - β - SiC和Ni - Ti - c - β - SiC催化剂在DRM中的性能。与以往在反应过程中使用MIR或不同载体的研究不同,该方法通过改变催化剂合成后MIR的暴露时间来调节Ni - β - SiC和Ni - Ti - c - β - SiC催化剂的金属-载体相互作用和结构性质。MIR后处理(10-25 s)使Ni -β-SiC催化剂的CH4转化率提高到65 %,CO2转化率提高到62 %,H₂/CO比提高到0.80,在20 H内性能稳定。对于ni - ti - c - β - sic, MIR(10-20 s)在20 h内保持了高达60% %的CH4转化率和58% %的CO2转化率,而未经处理的催化剂虽然最初较高,但很快失活。过多的MIR(30 s)降低了两种催化剂类型的性能,强调了对最佳暴露时间的需求。这些发现表明,合成后的MIR提供了一种可调的方法,通过控制金属载体相互作用的改性来提高Ni/SiC基DRM催化剂的活性和耐久性。这项工作为设计旨在温室气体利用和可持续合成气生产的稳健催化剂提供了新的见解,其活性和稳定性的增强与金属-载体相互作用的可控变化有关。
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引用次数: 0
Application of acid digestion-based total inorganic carbon measurement for carbonated cement-based materials 酸消化法测定总无机碳在碳酸水泥基材料中的应用
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1016/j.jcou.2025.103266
Ryo Kurihara , Luge Cheng , Ryusei Igami , Zhenzhen Wang , Abudushalamu Aili , Kiyuki Noto , Minako Tanaka , Haruka Takahashi , Ippei Maruyama
There is growing societal demand for methods to quantify the amount of CO₂ immobilized in cement-based materials. In this study, we compared and evaluated multiple analytical approaches: two different interpretation methods applied to thermogravimetric analysis (TGA) data conventionally used in this field, and two techniques widely adopted in soil science and related areas. The first of these involves heating the sample to release CO₂, which is then quantified using infrared absorption spectroscopy; the second involves dissolving carbonates in the sample using acid, with the evolved CO₂ gas similarly measured using infrared absorption. In carbonated cement pastes, when silica gel and carbonates are in close contact, CO₂ may be released at relatively low temperatures. This temperature range overlaps that of organic matter decomposition, which can complicate quantitative analyses using thermal methods. However, accurate quantification is feasible in systems with minimal organic content. During acid decomposition, silica gel may interfere with carbonate dissolution. Nevertheless, if the sample is sufficiently ground, an appropriate volume of the acid solution is used, and the dissolution time is properly managed under stirring conditions, this method offers a simple and practical means for CO₂ quantification.
社会对量化水泥基材料中固定二氧化碳量的方法的需求越来越大。在这项研究中,我们比较和评估了多种分析方法:两种不同的解释方法应用于该领域的热重分析(TGA)数据,以及两种在土壤科学和相关领域广泛采用的技术。第一种方法是加热样品以释放CO₂,然后使用红外吸收光谱对其进行量化;第二种方法是用酸溶解样品中的碳酸盐,同样用红外吸收法测量释放出的二氧化碳气体。在碳化水泥浆中,当硅胶和碳酸盐紧密接触时,在相对较低的温度下可能会释放CO₂。这个温度范围与有机物分解的温度范围重叠,这会使使用热方法进行定量分析复杂化。然而,在有机含量极低的系统中,精确的定量是可行的。在酸分解过程中,硅胶会干扰碳酸盐的溶解。然而,如果样品充分研磨,使用适当体积的酸溶液,并在搅拌条件下适当管理溶解时间,则该方法为CO₂定量提供了一种简单实用的手段。
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引用次数: 0
A dynamic and functional based reclassification review of carbon dioxide mitigation strategies 基于动态和功能的二氧化碳减缓战略重新分类审查
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1016/j.jcou.2025.103251
Ghida Mawassi, Alessandro Di Pretoro, Ludovic Montastruc
Although the decarbonization challenge consists of a macro-scale system dynamics problem, the majority of classifications and environmental analyses proposed in literature are usually focused on a single process-scale technology from a steady-state perspective, offering poor insights about the protracted impact of process and energy plants retrofitting over time. Since CO2 decumulation in the atmosphere is the outcome of both replacement and removal strategies, innovative long-term criteria could lead to a more effective classification and provide a more direct correlation between the selected strategy and the competitive operations. In this review article, the effectiveness and the sequestration time of the most established CO2 removal strategies are analyzed and quantified in detail with the purpose of reclassifying them according to carbon dioxide release delay and removal efficiency and to distinguish whether energy, chemical or transportation aspects are involved. In particular, the proposed ranking aims at detecting the best performing technologies to be implemented since the early design stage for the targeted application according to their long-term CO2 removal effectiveness. As a result of this research, the most effective contributions are given by the maximization of carbon-free energy use, bio-based raw materials and by the conversion of carbon dioxide into long-life chemical products.
尽管脱碳挑战包括宏观尺度的系统动力学问题,但文献中提出的大多数分类和环境分析通常从稳态的角度关注单一工艺规模的技术,对工艺和能源工厂随着时间的推移进行改造的长期影响缺乏深入的了解。由于大气中的二氧化碳减积是替代和清除战略的结果,创新的长期标准可能导致更有效的分类,并在选定的战略和竞争性业务之间提供更直接的联系。本文对目前最成熟的CO2去除策略的有效性和固存时间进行了详细的分析和量化,目的是根据二氧化碳释放延迟和去除效率对其进行重新分类,并区分是否涉及能源、化学或运输方面。特别是,拟议的排名旨在根据目标应用的长期二氧化碳去除效果,检测从早期设计阶段开始实施的性能最佳的技术。由于这项研究,最有效的贡献是通过最大限度地利用无碳能源、生物基原材料和将二氧化碳转化为长寿命的化学产品。
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引用次数: 0
Synergistic chemo-enzymatic formic acid disproportionation and biomolecular condensates for efficient amino acid production 协同化学-酶甲酸歧化和高效氨基酸生产的生物分子凝聚
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-05 DOI: 10.1016/j.jcou.2025.103269
Aocong Guan , Yin Gao , Minhui Wang , Jinglei Nie , Jianming Liu , An-Ping Zeng
Formic acid, which can be sustainably produced from CO₂ electroreduction, serves as a renewable liquid C₁ carrier for carbon recycling. However, its biological assimilation is fundamentally constrained by unfavorable thermodynamics and limited metabolic flux. Here, we develop an artificial and efficient pathway to transform formic acid into amino-acid glycine through integrating non-enzymatic formic acid disproportionation with biomolecular condensate-mediated enzyme organization, overcoming these limitations. We first employed amorphous bismuth chromate hydroxide to catalyze formic acid disproportionation, and investigated how amorphous catalyst impacts efficiency, finding that amorphous bismuth chromate hydroxide yield substantially higher catalytic activity and enable the production of formaldehyde at M concentrations alongside CO₂ from formic acid. This chemical step provides a strong thermodynamic driving force for subsequent enzymatic glycine synthesis. Furthermore, we employed liquid-liquid phase separation (LLPS) to create biomolecular condensates, spatially organizing enzymes like natural carboxysomes to enhance catalytic efficiency. This hybrid chemical-biological strategy enables thermodynamically favorable, high-flux glycine production, offering a paradigm for transcending biological thermodynamic constraints through abiotic-biotic synergy coupling with engineered enzyme compartmentalization.
甲酸是一种可再生的液态C₁载体,可通过CO₂电还原可持续生产。然而,它的生物同化从根本上受到不利的热力学和有限的代谢通量的限制。本研究通过将非酶甲酸歧化与生物分子凝聚物介导的酶组织相结合,开发了一种将甲酸转化为氨基酸甘氨酸的人工高效途径,克服了这些局限性。我们首先使用无定形氢氧化铬酸铋催化甲酸歧化,并研究了无定形催化剂对效率的影响,发现无定形氢氧化铬酸铋的催化活性大大提高,并且可以在M浓度下与CO 2一起从甲酸中生成甲醛。这一化学步骤为后续的酶促甘氨酸合成提供了强大的热力学驱动力。此外,我们采用液-液相分离(LLPS)技术创建生物分子凝聚体,在空间上组织酶,如天然羧体,以提高催化效率。这种化学-生物混合策略可以实现热力学有利的高通量甘氨酸生产,为通过非生物-生物协同作用与工程酶区隔化耦合超越生物热力学约束提供了范例。
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引用次数: 0
Valorization of carbon dioxide via the organic electro-refinery concept: Demonstrating the feasibility of a sustainable process 通过有机电精炼厂概念实现二氧化碳的增值:展示可持续过程的可行性
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-04 DOI: 10.1016/j.jcou.2025.103265
S. Maldonado , R. Garcia-Cervilla , G. Roa-Morales , R. Natividad , J. Lobato , M.A. Rodrigo
In this study, we present a successful demonstration of carbon dioxide transformation into carboxylate-rich solutions through a sequential process integrating biological and electrochemical technologies. The process comprises three main stages: (1) CO₂ fixation via algal cultivation, (2) electrochemical conversion of the algal biomass into carboxylates, and (3) separation and purification of the resulting acids using electrodialysis. Each stage was systematically evaluated to determine process efficiency and yield. First, atmospheric CO₂ was effectively fixed into algal biomass at varying cell retention times (2–10 days), with a 5-day retention time yielding the highest productivity, up to 37.65 mg day⁻¹ at an air flow rate of 4.1 L h⁻¹ . Shorter retention times led to biomass washout, limiting fixation efficiency. Second, the algal biomass was electrochemically transformed into carboxylate-containing solutions. The formation of these compounds followed a bimodal distribution: an initial release of native carboxylates from the algal matrix, followed by electrolytic generation via oxidation of organic matter, consistent with the organic electro-refinery concept. Acetate and malonate were predominantly associated with the first phase, while formate and oxalate were linked to the second. Finally, carboxylates were successfully recovered using electrodialysis with anion-exchange membranes. Recovery efficiency was strongly influenced by the applied current density, with up to 60 % of the carbon introduced via the algal suspension recovered as purified carboxylate solutions. These findings demonstrate the technical feasibility and promise of a fully solar-powered, integrated biological-electrochemical platform for CO₂ valorization, offering a novel and sustainable pathway for climate change mitigation.
在这项研究中,我们展示了通过结合生物和电化学技术的顺序过程将二氧化碳转化为富含羧酸盐的溶液的成功演示。该过程包括三个主要阶段:(1)通过藻类培养固定CO 2;(2)将藻类生物质电化学转化为羧酸;(3)使用电渗析分离和纯化所得酸。每个阶段都进行了系统评估,以确定工艺效率和收率。首先,在不同的细胞保留时间(2-10天)下,大气中的二氧化碳被有效地固定在藻类生物量中,5天的保留时间产生最高的生产力,高达37.65 mg天(⁻¹ ),空气流速为4.1 L h⁻¹ 。较短的滞留时间导致生物量流失,限制了固定效率。其次,将藻类生物质电化学转化为含羧酸的溶液。这些化合物的形成遵循双峰分布:最初从藻类基质中释放天然羧酸盐,然后通过有机物氧化产生电解,这与有机电精炼厂的概念一致。乙酸酯和丙二酸酯主要与第一相结合,甲酸酯和草酸酯主要与第二相结合。最后,利用阴离子交换膜进行电渗析,成功回收羧酸盐。回收效率受到施加电流密度的强烈影响,通过藻类悬浮液引入的碳中高达60% %作为纯化的羧酸盐溶液回收。这些发现证明了一种完全由太阳能供电的、集成的生物电化学平台用于二氧化碳增值的技术可行性和前景,为减缓气候变化提供了一种新的、可持续的途径。
{"title":"Valorization of carbon dioxide via the organic electro-refinery concept: Demonstrating the feasibility of a sustainable process","authors":"S. Maldonado ,&nbsp;R. Garcia-Cervilla ,&nbsp;G. Roa-Morales ,&nbsp;R. Natividad ,&nbsp;J. Lobato ,&nbsp;M.A. Rodrigo","doi":"10.1016/j.jcou.2025.103265","DOIUrl":"10.1016/j.jcou.2025.103265","url":null,"abstract":"<div><div>In this study, we present a successful demonstration of carbon dioxide transformation into carboxylate-rich solutions through a sequential process integrating biological and electrochemical technologies. The process comprises three main stages: (1) CO₂ fixation via algal cultivation, (2) electrochemical conversion of the algal biomass into carboxylates, and (3) separation and purification of the resulting acids using electrodialysis. Each stage was systematically evaluated to determine process efficiency and yield. First, atmospheric CO₂ was effectively fixed into algal biomass at varying cell retention times (2–10 days), with a 5-day retention time yielding the highest productivity, up to 37.65 mg day⁻¹ at an air flow rate of 4.1 L h⁻¹ . Shorter retention times led to biomass washout, limiting fixation efficiency. Second, the algal biomass was electrochemically transformed into carboxylate-containing solutions. The formation of these compounds followed a bimodal distribution: an initial release of native carboxylates from the algal matrix, followed by electrolytic generation via oxidation of organic matter, consistent with the organic electro-refinery concept. Acetate and malonate were predominantly associated with the first phase, while formate and oxalate were linked to the second. Finally, carboxylates were successfully recovered using electrodialysis with anion-exchange membranes. Recovery efficiency was strongly influenced by the applied current density, with up to 60 % of the carbon introduced via the algal suspension recovered as purified carboxylate solutions. These findings demonstrate the technical feasibility and promise of a fully solar-powered, integrated biological-electrochemical platform for CO₂ valorization, offering a novel and sustainable pathway for climate change mitigation.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103265"},"PeriodicalIF":8.4,"publicationDate":"2025-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145462503","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
Accelerated carbonation of ladle furnace slag: A dual approach to CO2 utilization and waste valorization in sustainable cement applications 钢包炉渣加速碳化:可持续水泥应用中二氧化碳利用和废物增值的双重途径
IF 8.4 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-04 DOI: 10.1016/j.jcou.2025.103267
Farah Kaddah , Ahmed Hamdy Abdelgawad , Ludovic F. Dumée , Nahla Al Amoodi , Imad Barsoum , Ahmed Alhajaj
The cement industry contributes nearly 8 % of global anthropogenic CO₂ emissions, largely driven by energy-intensive clinker production and limestone calcination. Innovative pathways to reduce this carbon footprint are critical for meeting global climate targets. This study explores the valorization of ladle furnace slag (LFS) through accelerated CO₂ carbonation, transforming it into a reactive supplementary cementitious material (SCM) that simultaneously enhances cement performance and sequesters CO₂. LFS was exposed to 100 % CO₂ for up to 72 h, achieving a CO₂ uptake of 3.3 g per 100 g slag. Incorporation of carbonated LFS at 25 % and 50 % replacement levels in cement pastes revealed significant improvements in hydration kinetics, microstructure, mechanical strength, and durability. Microstructural characterization identified the formation of nano-crystalline CaCO₃ polymorphs, which intensified pozzolanic reactivity and particle bonding. Compared to uncarbonated slag, carbonated LFS accelerated early hydration and enhanced long term strength exhibiting a 22.8 % compressive strength increase at 64 days for 25 % replacement. Reductions were observed in water absorption (7.8 %), porosity (5.2 %), and carbonation depth (17.7 %). These results demonstrate that CO₂ carbonation pretreatment not only captures carbon but also upgrades industrial waste into a high-performance, low-carbon SCM. This dual-function strategy aligns with circular economy principles and advances sustainable cement production through CO₂ utilization.
水泥行业贡献了全球近8 %的人为二氧化碳排放量,主要是由能源密集型熟料生产和石灰石煅烧驱动的。减少碳足迹的创新途径对于实现全球气候目标至关重要。本研究探讨了钢包炉渣(LFS)通过加速CO₂碳化的增值,将其转化为一种活性补充胶凝材料(SCM),同时提高水泥性能和封存CO₂。LFS暴露在100 % CO₂中长达72 h,每100 g炉渣的CO₂吸收率为3.3 g。在水泥浆中掺入25% %和50% %替代水平的碳化LFS,可以显著改善水化动力学、微观结构、机械强度和耐久性。微观结构表征发现纳米晶CaCO₃多晶态的形成,增强了火山灰反应性和颗粒键合。与未碳化的矿渣相比,碳化后的矿渣加速了早期水化,并提高了长期强度,在置换25% %的矿渣64天后,其抗压强度提高了22.8% %。吸水率(7.8 %)、孔隙率(5.2 %)和碳化深度(17.7 %)均有所降低。这些结果表明,CO₂碳化预处理不仅可以捕获碳,还可以将工业废物升级为高性能,低碳的SCM。这种双重功能战略符合循环经济原则,并通过二氧化碳的利用促进可持续水泥生产。
{"title":"Accelerated carbonation of ladle furnace slag: A dual approach to CO2 utilization and waste valorization in sustainable cement applications","authors":"Farah Kaddah ,&nbsp;Ahmed Hamdy Abdelgawad ,&nbsp;Ludovic F. Dumée ,&nbsp;Nahla Al Amoodi ,&nbsp;Imad Barsoum ,&nbsp;Ahmed Alhajaj","doi":"10.1016/j.jcou.2025.103267","DOIUrl":"10.1016/j.jcou.2025.103267","url":null,"abstract":"<div><div>The cement industry contributes nearly 8 % of global anthropogenic CO₂ emissions, largely driven by energy-intensive clinker production and limestone calcination. Innovative pathways to reduce this carbon footprint are critical for meeting global climate targets. This study explores the valorization of ladle furnace slag (LFS) through accelerated CO₂ carbonation, transforming it into a reactive supplementary cementitious material (SCM) that simultaneously enhances cement performance and sequesters CO₂. LFS was exposed to 100 % CO₂ for up to 72 h, achieving a CO₂ uptake of 3.3 g per 100 g slag. Incorporation of carbonated LFS at 25 % and 50 % replacement levels in cement pastes revealed significant improvements in hydration kinetics, microstructure, mechanical strength, and durability. Microstructural characterization identified the formation of nano-crystalline CaCO₃ polymorphs, which intensified pozzolanic reactivity and particle bonding. Compared to uncarbonated slag, carbonated LFS accelerated early hydration and enhanced long term strength exhibiting a 22.8 % compressive strength increase at 64 days for 25 % replacement. Reductions were observed in water absorption (7.8 %), porosity (5.2 %), and carbonation depth (17.7 %). These results demonstrate that CO₂ carbonation pretreatment not only captures carbon but also upgrades industrial waste into a high-performance, low-carbon SCM. This dual-function strategy aligns with circular economy principles and advances sustainable cement production through CO₂ utilization.</div></div>","PeriodicalId":350,"journal":{"name":"Journal of CO2 Utilization","volume":"102 ","pages":"Article 103267"},"PeriodicalIF":8.4,"publicationDate":"2025-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145462495","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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Journal of CO2 Utilization
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