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Continuous CO2 capture using a hollow fiber membrane contactor with stripper regeneration: Bench-scale validation with amino acid salt–piperazine absorbents 连续CO2捕获使用中空纤维膜接触器与脱提器再生:氨基酸盐-哌嗪吸收剂的实验规模验证
Pub Date : 2026-01-17 DOI: 10.1016/j.ccst.2026.100573
Hyunji Lim , Kwanghwi Kim , Hyun Sic Park , Jo Hong Kang , Jinwon Park , Hojun Song
Membrane contactor technologies offer a promising solution for CO2 capture; however, their optimization remains challenging. This study explored the CO2 absorption and desorption performances in a hybrid process involving a hollow fiber membrane contactor (HFMC) and a stripping tower in a bench-scale system. Three absorbents [2.5 M monoethanolamine (MEA), potassium serinate + piperazine (PSZ), and potassium alaninate + piperazine (PAZ)] were tested at total absorbent molarity under varying liquid flow rates to evaluate their CO2 removal efficiencies, absorption fluxes, and overall mass transfer coefficients. The results showed that PAZ exhibited the highest CO2 capture performance, while also significantly reducing the regeneration energy and membrane wetting. The PAZ absorbent maintained a stable performance during simultaneous operation, with a 73 % reduction in crossover volume and a 31 % decrease in the regeneration energy compared to MEA. The membrane contactor process demonstrated enhanced characteristics compared to a conventional packed column under similar gas flow rates, with a four times higher CO2 absorption rate and a 79 % smaller unit volume. Furthermore, long-term oxidative degradation tests confirmed the durability of the PAZ absorbent. Overall, this study demonstrates the potential of combining HFMCs with optimized PAZ absorbents to enhance the CO2 capture efficiency and minimize operational challenges, leading to a more compact and efficient carbon capture process.
膜接触器技术为二氧化碳捕获提供了一个很有前途的解决方案;然而,它们的优化仍然具有挑战性。研究了中空纤维膜接触器(HFMC)与汽提塔混合工艺在实验系统中的CO2吸收和解吸性能。在不同液体流速下测试了三种吸收剂[2.5 M单乙醇胺(MEA)、丝氨酸钾+哌嗪(PSZ)和丙氨酸钾+哌嗪(PAZ)]的总吸附剂摩尔浓度,以评估它们的CO2去除效率、吸收通量和总传质系数。结果表明,PAZ具有最高的CO2捕获性能,同时也显著降低了再生能量和膜润湿性。与MEA相比,PAZ吸收剂在同时运行时保持稳定的性能,交叉体积减少73%,再生能量减少31%。在相同的气体流速下,膜接触器工艺与传统填料塔相比,具有更强的特性,二氧化碳吸收率提高了4倍,单位体积减小了79%。此外,长期氧化降解试验证实了PAZ吸附剂的耐久性。总体而言,该研究表明,将hfmc与优化的PAZ吸收剂相结合,可以提高二氧化碳捕集效率,最大限度地减少操作挑战,从而实现更紧凑、更高效的碳捕集过程。
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引用次数: 0
Persulfate–derived porous wollastonite granules for accelerated CO2 mineralization and suitability for aggregate applications 过硫酸盐衍生多孔硅灰石颗粒加速二氧化碳矿化和适合骨料应用
Pub Date : 2026-01-16 DOI: 10.1016/j.ccst.2026.100571
Prince Allah, Tero Luukkonen, Paivo Kinnunen, Priyadharshini Perumal
Mineral carbonation technology is a promising solution for CO2 capture and utilization. To achieve large scale application of the technology, the challenges related to CO2 diffusion and passivation by carbonate precipitation must be overcome. In this work, we demonstrate a route to high volume CO2 capture by granulation and carbonation using wollastonite, polyvinyl alcohol (pva) and potassium persulfate. The wollastonite powder was granulated with 10% pva solution, incorporating 10–100 wt% of granulation fluid of potassium persulfate as pore–forming agent. The utility of some granules was extended by esterification reaction in citric acid solution. The granules were carbonated in a pressured reactor (10 bar, 100 °C) and the influence of pore–forming amount on carbonate passivation and CO2 diffusion was studied by thermogravimetry, optical, electron microscopy and N2 adsorption. The experiments revealed that 20% persulfate produced highly porous granules with an interconnected pore structure that reduced carbonate passivation and captured the highest amount of CO2 (44mol%). Comparatively, mix designs with 0, 10 and 100 wt% persulfate showed low carbonation due to poor CO2 diffusion attributed to surface passivation by carbonates and sulfates. Additionally, pore structure and surface modelling using Frankel–Halsey–Hill (FHH) fractal analysis concludes that 20% persulfate in both fresh and esterified granules produced a less tortuous and uniform pore structure with high interconnectivity, aiding CO2 diffusion within the granules which resulted in high amount of carbonation products while preventing passivation. After carbonation, the aggregates maintained high strength and light weight, confirming their high potential as a high-volume CO2 negative artificial lightweight aggregate in construction.
矿物碳酸化技术是一种很有前途的二氧化碳捕获和利用解决方案。为了实现该技术的大规模应用,必须克服二氧化碳扩散和碳酸盐沉淀钝化的挑战。在这项工作中,我们展示了一种利用硅灰石、聚乙烯醇(pva)和过硫酸钾进行造粒和碳化的方法来捕获大量二氧化碳的途径。硅灰石粉用10%的聚乙烯醇溶液造粒,加入10 - 100wt %的过硫酸钾造粒液作成孔剂。通过在柠檬酸溶液中酯化反应,扩大了某些颗粒的使用范围。在压力反应器(10 bar, 100℃)中碳化颗粒,通过热重、光学、电子显微镜和N2吸附研究成孔量对碳酸盐钝化和CO2扩散的影响。实验表明,20%的过硫酸盐产生了具有互连孔结构的高多孔颗粒,减少了碳酸盐钝化,并捕获了最高量的CO2 (44mol%)。相比之下,含有0、10%和100%过硫酸盐的混合物设计显示出低碳化,这是由于碳酸盐和硫酸盐表面钝化导致二氧化碳扩散不良。此外,利用Frankel-Halsey-Hill (FHH)分形分析进行的孔隙结构和表面建模得出结论,20%的过硫酸盐在新鲜颗粒和酯化颗粒中产生的孔隙结构不那么弯曲和均匀,具有较高的互联性,有助于二氧化碳在颗粒内的扩散,从而产生大量的碳化产物,同时防止钝化。碳化后,骨料保持了高强度和轻重量,证实了它们在建筑中作为大体积负二氧化碳人工轻质骨料的巨大潜力。
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引用次数: 0
Effect of cation’s alkyl chain length of imidazolium-driven PVDF-based supported ionic liquid membranes on the CO2 separation performance from biogas and flue gas 咪唑驱动pvdf基负载离子液体膜阳离子烷基链长对沼气和烟气CO2分离性能的影响
Pub Date : 2026-01-16 DOI: 10.1016/j.ccst.2026.100572
G. Marco-Velasco, V. Martínez-Soria, M. Izquierdo, A. Cháfer, J.D. Badia-Valiente
This study investigates the impact of the alkyl chain length in imidazolium-based ILs on SILMs using poly(vinylidene fluoride) (PVDF) as a polymer substrate on the membrane’s physicochemical properties and CO2 separation performance from CO2/CH4 and CO2/N2 gas mixtures. Particularly, 1-Ethyl, 1-Butyl and 1-Hexyl 3-methylimidazolium bis(trifluoromethylsulfonyl)imide, i.e. [EMIM][NTf2], [BMIM][NTf2], and [HMIM][NTf2]-based SILMs, were assessed. Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM) and energy dispersive X-ray (EDX) confirmed and quantified the presence of ILs within the polymeric matrix, while differential scanning calorimetry (DSC) suggested larger electrostatic interactions for shorter alkyl chains on imidazolium cations. CO2, CH4 and N2 permeability of each SILM were assessed by single-gas permeability tests and their CO2/N2 and CO2/CH4 selectivity were achieved. ILs with shorter alkyl chain presented stronger interactions with CO2 molecules. [EMIM][NTf₂] SILM exhibited the highest single-gas CO₂ permeability (357.0 Barrer), CO2/CH4 selectivity (αCO2/CH4 =23.5) and CO2/N2 selectivity (αCO2/N2 =16.4), which were competitive when benchmarked in an upper bound plot. Afterwards, this SILM was tested in extended experiments under dry and humid conditions (≥ 90 h each), in which CO2 feed composition was modified between CO2/CH4 50/50 %v/v and 25/75 %v/v. CH4 permeability increased as its proportion in the feed was reduced (from 15.4 Barrer using 100 %v/v CH4 to 20.5 and 19.9 Barrer when CH4 was fed at 50 %v/v or higher, under dry and humid conditions, respectively), affecting CO2/CH4 selectivity (from ∼24 for single gas to ∼17 and ∼19 in dry and humid experiments, respectively), remaining competitive regarding the technological benchmarking.
本文研究了以聚偏氟乙烯(PVDF)为聚合物底物的咪唑基膜的烷基链长度对膜的物理化学性能和CO2/CH4和CO2/N2混合气体分离性能的影响。特别是对1-乙基、1-丁基和1-己基3-甲基咪唑双(三氟甲基磺酰基)亚胺,即[EMIM][NTf2]、[BMIM][NTf2]和[HMIM][NTf2]基silm进行了评估。傅里叶变换红外光谱(FTIR)、扫描电镜(SEM)和能量色散x射线(EDX)证实并量化了聚合物基体中il的存在,而差示扫描量热法(DSC)表明咪唑阳离子上较短的烷基链存在较大的静电相互作用。通过单气体渗透性测试,评估了各SILM的CO2、CH4和N2渗透率,获得了其CO2/N2和CO2/CH4选择性。烷基链较短的ILs与CO2分子的相互作用较强。[EMIM][NTf₂]SILM表现出最高的单气CO₂渗透率(357.0 Barrer), CO2/CH4选择性(αCO2/CH4 =23.5)和CO2/N2选择性(αCO2/N2 =16.4),在上界基准图中具有竞争性。然后,在干湿条件下(≥90 h)对该SILM进行扩展试验,其中CO2饲料成分在CO2/CH4 50/ 50% v/v和25/ 75% v/v之间进行改性。CH4渗透率随着其在饲料中所占比例的降低而增加(在干燥和潮湿条件下,分别从100% v/v CH4时的15.4 Barrer降至50% v/v或更高CH4时的20.5 Barrer和19.9 Barrer),影响CO2/CH4的选择性(在干燥和潮湿条件下,分别从单一气体的~ 24降至干燥和潮湿条件下的~ 17和~ 19),在技术基准方面保持竞争力。
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引用次数: 0
Investigating carbon sequestration in cementitious mortars with low-carbon binders and carbonated water 研究低碳粘结剂和碳酸水对水泥砂浆固碳的影响
Pub Date : 2026-01-09 DOI: 10.1016/j.ccst.2026.100570
Aswathy Rajendran, Sripriya Rengaraju, Abir Al-Tabbaa
The use of carbonated water in cementitious systems as a carbon sequestration strategy is promising, offering operational simplicity and high CO2 binding efficiency compared to approaches such as gaseous CO2 injection and carbonation curing. However, its application in low-carbon cement systems, particularly emerging binders such as limestone calcined clay cement (LC3), remains underexplored. As the shift to low-carbon binders is critical for reducing embodied carbon in cement, it is essential to understand their interactions with carbonated water, given their distinct reactivity, pH evolution, and fresh-state behaviour. This study systematically investigates the effects of carbonated water on conventional low-carbon binders (Slag-50% and Slag-80%), emerging LC3, and OPC mortars. Evaluations covered fresh-state properties, mechanical performance, durability (sorptivity and porosity), and microstructural evolution at early and later ages. Results show the strongest interaction of carbonate ions with C3A and its hydration products, with CO2 binding governed by the nature of early hydrates and pH conditions. Contrary to the hypothesis that high-calcium systems such as OPC are most favourable for CO2 binding, they exhibited reduced strength and durability. In contrast, LC3 and Slag-50% demonstrated the greatest benefits, with improved CO2 binding, shortened setting times, enhanced strength and reduced sorptivity and porosity. Microstructural analysis confirmed CO2 binding predominantly influenced calcium-silicate-hydrate gels with minimal calcite formation. Overall, carbonated water emerges as a practical pathway to improve performance while enabling additional CO2 binding in LC3 and slag-50% cement systems, reinforcing their superior potential for carbon sequestration to OPC.
在胶凝系统中使用碳酸水作为固碳策略是很有前途的,与气体二氧化碳注入和碳化固化等方法相比,它具有操作简单和高二氧化碳结合效率的优点。然而,它在低碳水泥体系中的应用,特别是新兴的粘结剂,如石灰石煅烧粘土水泥(LC3),仍未得到充分的探索。由于向低碳粘结剂的转变对于减少水泥中的隐含碳至关重要,因此考虑到它们独特的反应性、pH值演变和新鲜状态行为,了解它们与碳酸水的相互作用至关重要。本研究系统地研究了碳酸水对传统低碳粘结剂(矿渣-50%和矿渣-80%)、新兴LC3和OPC砂浆的影响。评估内容包括新鲜状态特性、机械性能、耐久性(吸附性和孔隙率)以及早期和后期的微观结构演变。结果表明,碳酸盐离子与C3A及其水化产物的相互作用最强,其与CO2的结合受早期水合物性质和pH条件的制约。与高钙体系(如OPC)最有利于二氧化碳结合的假设相反,它们表现出强度和耐久性降低。相比之下,LC3和炉渣-50%表现出最大的效益,改善了CO2结合,缩短了凝结时间,提高了强度,降低了吸附率和孔隙率。微观结构分析证实,二氧化碳结合主要影响硅酸钙水合物凝胶,方解石形成较少。总的来说,碳酸水是一种实用的方法,可以提高性能,同时在LC3和矿渣-50%的水泥体系中增加二氧化碳的结合,增强其对OPC的碳封存潜力。
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引用次数: 0
Additive manufacturing of architected Ca(OH)2 monoliths for accelerated CO2 mineralization 用于加速CO2矿化的结构Ca(OH)2单体的增材制造
Pub Date : 2026-01-07 DOI: 10.1016/j.ccst.2026.100568
Injun Park , Sunwoo Kim , Byeongju Jeon , Huiryung Heo , Siyoung Q. Choi , Jay H. Lee , Dong-Yeun Koh
Effective CCU technologies demand robust, scalable sorbents with high CO2 selectivity and capacity. While calcium hydroxide (Ca(OH)2) offers high CO2 uptake via mineral carbonation, its practical application is hindered by slow reaction kinetics and difficulties in forming mechanically stable, structured beds. Here, we report a direct ink writing (DIW) approach to fabricate 3D-printed Ca(OH)2 monoliths using water-based inks formulated with carboxymethyl cellulose (CMC). Under humid conditions (RH95, 1–10 mol % CO2), the monolith achieves >99 % conversion to calcium carbonate, with similarly strong performance maintained at 400 ppm CO2 relevant to direct air capture (DAC). The structured sorbent also exhibits extremely low pressure drop (∼2 Pa/cm), making it suitable for scaled-up applications. A techno-economic analysis (TEA) for the DAC case, incorporating parallel nozzle printing, shows that the levelized cost of capture (LCOC) can be reduced to 339 US$/tCO2, with break-even scenarios attainable through carbon subsidies or high-value reuse of the monolith reuse. Overall, this work establishes a dry, scalable pathway for fabricating reactive structured Ca(OH)2 sorbents for CCU applications.
有效的CCU技术需要具有高CO2选择性和容量的强大,可扩展的吸附剂。虽然氢氧化钙(Ca(OH)2)通过矿物碳酸化提供了高的二氧化碳吸收率,但其实际应用受到反应动力学缓慢和难以形成机械稳定的结构层的阻碍。在这里,我们报告了一种直接墨水书写(DIW)方法,使用羧甲基纤维素(CMC)配制的水性油墨来制造3d打印的Ca(OH)2单体。在潮湿的条件下(RH95, 1-10 mol %的二氧化碳),整体实现99%的转化为碳酸钙,与直接空气捕获(DAC)相关的400 ppm二氧化碳保持同样强大的性能。结构吸附剂还具有极低的压降(~ 2 Pa/cm),使其适合扩大应用。采用平行喷嘴印刷的DAC案例的技术经济分析(TEA)表明,捕集的平准化成本(LCOC)可降至每吨二氧化碳339美元,通过碳补贴或单体再利用的高价值再利用可实现收支平衡。总的来说,这项工作建立了一种干燥的、可扩展的途径,用于制造用于CCU应用的活性结构Ca(OH)2吸附剂。
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引用次数: 0
Warm gas carbon dioxide capture from the anode off-gas in solid oxide fuel cell-gas turbine hybrid power generation systems: A technoeconomic investigation considering economies-of-scale 固体氧化物燃料电池-燃气轮机混合发电系统中阳极废气的热气体二氧化碳捕获:考虑规模经济的技术经济研究
Pub Date : 2026-01-07 DOI: 10.1016/j.ccst.2025.100562
Yee Lee Chen , Praneet Atul Chotalia , Fabian Rosner
The thermodynamic and economic performance of a warm gas pressure swing adsorption (PSA) technology for carbon dioxide (CO2) capture directly from the anode off-gas in a solid oxide fuel cell (SOFC)-gas turbine (GT) hybrid power generation system is investigated. Warm gas CO2 capture provides advantages over ambient temperature CO2 capture by retaining water vapor in the anode off-gas, simplifying heat integration and preserving higher mass flows through the turbine, maximizing energy efficiency and downstream power generation. Four cases of natural gas (NG)-powered SOFC-GT hybrid plants are compared: 10 MW and 50 MW systems without carbon capture, and 50 MW and 100 MW systems with carbon capture. At the 50 MW scale, the efficiency of the system without carbon capture achieves 75.32 %-LHV and the system with carbon capture achieves 68.22 %-LHV. This decrease in efficiency is governed by the loss of mass that moves through the turbine and the energy penalty associated with the heat needed for regeneration. The cost-of-capture of the warm gas PSA system is $74.87 (with TS&M) or $46.18 (without TS&M) per metric tonne of CO2. Efficiency improvements due to scaleup are marginal, nevertheless, the larger-scale hybrids are shown to be substantially more cost-effective. Comparing the 50 MW hybrid with carbon capture to the 100 MW hybrid, the specific plant cost decreases by 4.7 % and the cost of electricity decreases by 5.4 %. The analysis establishes warm gas PSA as a promising approach for integrating efficient and economic carbon capture into SOFC-GT hybrid power generation systems.
研究了固体氧化物燃料电池(SOFC)-燃气轮机(GT)混合发电系统中暖气变压吸附(PSA)技术直接从阳极废气中捕集二氧化碳(CO2)的热力学和经济性能。通过将水蒸气保留在阳极废气中,简化热集成并保持通过涡轮机的更高质量流量,最大限度地提高能源效率和下游发电,热气体CO2捕获比环境温度CO2捕获具有优势。对四种天然气(NG)驱动的SOFC-GT混合电厂进行了比较:无碳捕集的10兆瓦和50兆瓦系统,以及有碳捕集的50兆瓦和100兆瓦系统。在50 MW规模下,无碳捕集系统的效率达到75.32% -LHV,有碳捕集系统的效率达到68.22% -LHV。这种效率的下降是由通过涡轮机的质量损失和与再生所需的热量相关的能量损失控制的。暖气体PSA系统的捕获成本为每公吨二氧化碳74.87美元(含TS&;M)或46.18美元(不含TS&;M)。由于规模扩大而带来的效率提高是微不足道的,然而,大规模混合动力车的成本效益大大提高。将带有碳捕获的50兆瓦混合动力与100兆瓦混合动力相比,具体工厂成本降低了4.7%,电力成本降低了5.4%。分析表明,暖气PSA是一种很有前途的方法,可以将高效、经济的碳捕获整合到SOFC-GT混合发电系统中。
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引用次数: 0
Comparative environmental techno-economic assessments (eTEAs) of onboard amine-based carbon capture and boil-off gas handling systems on LCO2 carriers LCO2载体上基于胺的碳捕获和蒸发气体处理系统的比较环境技术经济评估(eTEAs)
Pub Date : 2026-01-07 DOI: 10.1016/j.ccst.2026.100569
Hongkyoung Shin , Juyoung Oh , Yunju Jeon , Youngsub Lim , Thomas A. Adams II
The continuous increase in greenhouse gas (GHG) emissions and the strengthening of environmental regulations have brought Carbon Capture, Utilization, and Storage (CCUS) technology into focus. Most liquefied carbon dioxide carriers (LCO2Cs) employ liquefied natural gas (LNG) propulsion, but they still emit significant GHG emissions, highlighting the need for further reduction. While boil-off gas (BOG) handling is essential for long-distance LCO2C operations, no studies have examined onboard carbon capture and storage (OCCS) systems integrated with BOG handling systems. This study evaluates five operational cases—BOG re-liquefaction (RLIQ), OCCS, purge gas recapture, and their combinations—to assess the GHG reduction and economic feasibility of LCO2Cs. Although standalone RLIQ and OCCS showed similar reduction rates (29% and 30%), the avoidance cost of OCCS alone was more than two times higher. Integrating BOG RLIQ, OCCS, and purge recirculation achieved up to 69% well-to-wake emission reduction with an avoidance cost of $355.9/tCO₂eq. Therefore, integrating OCCS with BOG RLIQ is the most effective approach for LCO2Cs. Despite limited competitiveness under current low carbon tax levels, the avoidance cost of $320–416/tCO₂eq remains favorable compared with other low-carbon technologies such as direct air capture ($500–1100/tCO₂eq).
温室气体(GHG)排放的持续增加和环境法规的加强使碳捕集、利用和封存(CCUS)技术成为人们关注的焦点。大多数液化二氧化碳运输船(LCO2Cs)采用液化天然气(LNG)推进,但它们仍会排放大量温室气体,因此需要进一步减排。虽然蒸发气(BOG)处理对于长距离LCO2C作业至关重要,但目前还没有研究将BOG处理系统集成在船上的碳捕获和储存(OCCS)系统中。本研究评估了五种操作案例——bog再液化(RLIQ)、OCCS、吹扫气体再捕获及其组合——以评估LCO2Cs的温室气体减排和经济可行性。虽然单独的RLIQ和OCCS显示出相似的降低率(29%和30%),但单独的OCCS的避免成本高出两倍多。整合BOG RLIQ、OCCS和吹扫再循环,可将井尾排放减少69%,避免成本为355.9美元/tCO₂当量。因此,将OCCS与BOG RLIQ集成是lco2c最有效的方法。尽管在目前的低碳税水平下竞争力有限,但与直接空气捕获(500-1100美元/tCO₂当量)等其他低碳技术相比,320-416美元/tCO₂当量的避免成本仍然是有利的。
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引用次数: 0
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
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Carbon Capture Science & Technology
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