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Breakthroughs in CH4 capture technologies: Key to reducing fugitive methane emissions in the energy sector 甲烷捕集技术的突破:减少能源行业甲烷散逸性排放的关键
Pub Date : 2024-11-05 DOI: 10.1016/j.ccst.2024.100316
Wenkang Deng , Xiaofeng Xie , Yalou Guo , Guoping Hu
A series of negative impacts caused by greenhouse gas emissions have driven mankind to look for a more efficient and economical strategy to reduce emissions. Methane is the second most abundant anthropogenic greenhouse gas, and implementing cost-effective technologies to reduce its emissions is a crucial pathway toward achieving the milestones outlined in the Paris Agreement. The energy sector has a greater potential for methane emission reductions than other sectors, such as (agriculture and waste) with 75 % reductions achievable by 2050 using existing technologies. Capturing and utilizing fugitive methane from the energy sector could offset the cost of emission reductions to some extent. We analyzed existing methane abatement technologies such as leak detection and repair, flaring, technology standards, and methane capture technologies and found that there are well-established solutions for methane leakage at medium and high concentrations. However, capturing methane from low-concentration sources to meet transportation or utilization requirements remains a significant technical challenge, highlighting the need for advances in low-grade methane enrichment technologies. Adsorption technology has been regarded as a promising methodology for methane capture in recent decades due to various advantages such as high flexibility, low capital investment and energy consumption, and a well-established technological framework. This review provides an overview of recent methane emission trends and prevalent methane abatement strategies, offering a brief analysis of the merits and drawbacks associated with existing methane capture technologies for industrial applications. We analyze the current methane emission reduction policies from major economies and identify a gap between proposed policies and practical actions, suggesting that constructing methane detection systems and developing low-concentration methane capture technologies is a key approach to closing the gap.
温室气体排放造成的一系列负面影响促使人类寻找更高效、更经济的减排策略。甲烷是第二大最丰富的人为温室气体,实施具有成本效益的技术来减少甲烷排放是实现《巴黎协定》所列阶段性目标的重要途径。与其他部门(如农业和废物处理)相比,能源部门的甲烷减排潜力更大,利用现有技术到 2050 年可实现 75% 的减排量。捕获和利用能源部门的逸散甲烷可在一定程度上抵消减排成本。我们分析了现有的甲烷减排技术,如泄漏检测和修复、燃烧、技术标准和甲烷捕集技术,发现对于中高浓度的甲烷泄漏已有成熟的解决方案。然而,从低浓度来源捕获甲烷以满足运输或利用要求仍然是一项重大的技术挑战,这凸显了低品位甲烷富集技术进步的必要性。近几十年来,吸附技术一直被认为是一种很有前景的甲烷捕集方法,因为它具有各种优势,如灵活性高、资本投资和能耗低以及技术框架完善等。本综述概述了最近的甲烷排放趋势和流行的甲烷减排策略,简要分析了工业应用中现有甲烷捕集技术的优缺点。我们分析了主要经济体当前的甲烷减排政策,并指出了拟议政策与实际行动之间的差距,建议构建甲烷检测系统和开发低浓度甲烷捕获技术是缩小差距的关键方法。
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引用次数: 0
Thermal characterization and moisture adsorption performance of calcium alginate hydrogel/silica gel/polyvinylpyrrolidone/expanded graphite composite desiccant 海藻酸钙水凝胶/硅胶/聚乙烯吡咯烷酮/膨胀石墨复合干燥剂的热特性和吸湿性能
Pub Date : 2024-11-04 DOI: 10.1016/j.ccst.2024.100323
Xin Xiao , Zhengliang Han , Yunfeng Wang , Ming Li
Solid desiccant dehumidification system can use low-grade energy for regeneration process and reduce the electrical energy consumption, thus saving energy and reducing carbon emissions. The choice of desiccant can significantly affect the dehumidification performance of the system. In the present study, the composite desiccant was synthesized by adding silica gel (SG), polyvinylpyrrolidone (PVP) and expanded graphite (EG) with calcium alginate hydrogel (CAH) as the matrix, named CAH/SG/EG. Subsequently, the characteristics of the samples were analyzed, and a dehumidification system was built to reveal the effects of different working conditions on the dehumidification performances. The results show that CAH/SG/20 wt.% EG has the optimal adsorption kinetics among all samples. Its moisture adsorption capacity reaches up to 1.009 g/g at 25 °C and 70 % relative humidity (RH), and its adsorption rate is 0.0179 g/(g·min). Especially, its moisture adsorption capacity can still reach 0.44 g/g at 30 % RH, showing a good adsorption capacity at lower RH. Simultaneously, the thermal conductivity of composites gradually increases from 0.449 W/(m·K) to 0.716 W/(m·K) with the addition of EG, increasing by about 60 %. In addition, the dehumidification performance of CAH/SG/20 wt.% EG is higher than that of CAH/SG, and the dehumidification performance of the system shows an ascending, descending and descending trends with the increase of inlet air moisture content, inlet air temperature and inlet air flow, respectively.
固体干燥剂除湿系统可以利用低品位能源进行再生处理,减少电能消耗,从而节约能源,减少碳排放。干燥剂的选择会极大地影响系统的除湿性能。本研究以海藻酸钙水凝胶(CAH)为基质,加入硅胶(SG)、聚乙烯吡咯烷酮(PVP)和膨胀石墨(EG),合成了复合干燥剂,命名为 CAH/SG/EG。随后,对样品的特性进行了分析,并建立了一个除湿系统,以揭示不同工作条件对除湿性能的影响。结果表明,在所有样品中,CAH/SG/20 wt.% EG 具有最佳的吸附动力学。在 25 °C、70 % 相对湿度(RH)条件下,其吸湿能力高达 1.009 g/g,吸湿率为 0.0179 g/(g-min)。特别是在相对湿度为 30% 时,其水分吸附能力仍能达到 0.44 g/g,显示出在较低相对湿度下也有很好的吸附能力。同时,随着 EG 的添加,复合材料的导热系数从 0.449 W/(m-K) 逐渐增加到 0.716 W/(m-K),增加了约 60%。此外,CAH/SG/20 wt.% EG 的除湿性能高于 CAH/SG,而且系统的除湿性能随着进气含湿量、进气温度和进气流量的增加分别呈上升、下降和下降趋势。
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引用次数: 0
Green solvents assisted de-novo synthesis and defect-engineered UiO-66 for improved CO2 adsorption and kinetics- experimental and DFT approach 实验和 DFT 方法:绿色溶剂辅助的脱嵌合成和缺陷工程 UiO-66,用于改善二氧化碳吸附和动力学性能
Pub Date : 2024-10-31 DOI: 10.1016/j.ccst.2024.100335
Saleem Nawaz Khan , Ming Zhao
The CO2 concentration in the atmosphere is increasing at an alarming rate, which is causing distress to human society and the natural environment. Adsorption is one of the most widely used methods of removing CO2 from flue gases, which reduces its adverse effects on our environment. For adsorption purposes, a facile green solvent-assisted de-novo synthesis approach was developed to construct a UiO-66′s structure to target CO2 at low pressure due to the partial pressure of CO2 in flue gases in the atmosphere (0.01⁓0.02 MPa). In the de-novo synthesis approach, a combination of various types of modulators and deep eutectic solvents (DES) are utilized to graft structural defects and induce quantitative and dispersive deep eutectic solvents onto the UiO-66 structure, respectively. The green solvent-assisted de-novo synthesis approach helped to tune all three structural parameters and preserve extra open metal sites (Lewis acid and Bronsted basis sites) with active NH2 and OH groups for improved CO2 adsorption and kinetics under flue gas conditions (CO2/N2=15/85 %). In comparison to the parent UiO-66, de-novo synthesized ChClPropx5@UiO-66 showed increased CO2 uptake (65.04 mg g-1) by 73 % at 0.15 bar and 25 °C, and the cyclic capacity remained almost similar over 10 consecutive cycles with an almost 94 % retention rate. After 3 times of regeneration at 105 °C under N2 atmosphere, the sample reserved almost similar adsorption capacity and could be recycled without dropping CO2 uptake. The strong and rapid interaction between guest CO2 and de-novo synthesized UiO-66 was confirmed by pseudo-first-order and second-order kinetics with reaction rate constants of 0.00026 and 0.00259, respectively. Furthermore, through periodic Density Functional Theory (DFT) calculations, a variety of linker defects are engineered onto the UiO-66 structure to preserve more open metal sites. For each of the engineering defects, free energies, adsorption energies, and the interaction of CO2 molecules on defect structures with bond length (Ɩ, Å) and bond angle (θ˚) are calculated for the most stable structures of UiO-66.
大气中的二氧化碳浓度正在以惊人的速度增加,这给人类社会和自然环境造成了困扰。吸附是最广泛使用的从烟气中去除二氧化碳的方法之一,它可以减少二氧化碳对环境的不利影响。由于大气中烟气中的二氧化碳分压(0.01⁓0.02 MPa)较低,为了达到吸附目的,研究人员开发了一种简便的绿色溶剂辅助从头合成方法来构建 UiO-66′s 结构,从而在低压下吸附二氧化碳。在脱嵌合成方法中,利用各种类型的调制剂和深共晶溶剂(DES)的组合,分别在 UiO-66 结构上接枝结构缺陷和诱导定量和分散深共晶溶剂。这种绿色溶剂辅助的去重合成方法有助于调整所有三个结构参数,并保留具有活性 NH2 和 OH 基团的额外开放金属位点(路易斯酸和勃朗斯特基位点),从而改善烟道气条件(CO2/N2=15/85%)下的二氧化碳吸附和动力学性能。与母体 UiO-66 相比,新合成的 ChClPropx5@UiO-66 在 0.15 巴和 25 °C条件下的二氧化碳吸附量(65.04 mg g-1)提高了 73%,并且在连续 10 个循环中的循环容量几乎保持不变,保留率接近 94%。在 105 °C、氮气环境下再生 3 次后,样品保留了几乎相似的吸附容量,并且可以循环使用而不会降低二氧化碳吸附量。伪一阶和二阶动力学证实了客体 CO2 与新合成的 UiO-66 之间强烈而快速的相互作用,反应速率常数分别为 0.00026 和 0.00259。此外,通过周期性密度泛函理论(DFT)计算,还在 UiO-66 结构上设计了多种链接缺陷,以保留更多开放的金属位点。针对每种工程缺陷,都计算出了 UiO-66 最稳定结构的自由能、吸附能以及二氧化碳分子在缺陷结构上与键长(Ɩ, Å)和键角(θ˚)的相互作用。
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引用次数: 0
CO2 absorption-desorption cycles: Progress, gaps, and future 二氧化碳吸收-解吸循环:进展、差距和未来
Pub Date : 2024-10-30 DOI: 10.1016/j.ccst.2024.100325
Tohid N. Borhani , Mohammad Reza Abbasi , Morteza Hosseinpour , Mohsen Salimi , Morteza Afkhamipour , Eni Oko , Kyra Sedransk Campbell , Navid Kahllaghi
In order to control global warming and CO2 emissions to the atmosphere, carbon capture from the carbon production source is considered the short- to midterm solution. The CO2 absorption-desorption process is recognised as a mature process that has been implemented for many years. However, this process has several weaknesses, such as the considerable energy requirements for regeneration in the desorber unit and degradation of solvent when using amine solutions. In this study, we examine several elements of absorption-desorption cycles for CO2 capture. This includes modelling, experimentation categorised by the unit operation employed, techno-economic analysis, optimisation, control strategies, and life cycle assessments. It discusses steady-state, dynamic, and data-driven based models, along with a selection of experimental studies conducted at the laboratory scale, detailing solvents used, column characteristics, and equipment specifications. Furthermore, it examines optimisation techniques, techno-economic assessments (TEA), and industrial applications, categorising them into power sectors and industries, and comparing their costs and energy requirements for carbon capture processes. Additionally, different control strategies for absorption-desorption systems are reviewed, compared, and discussed. Life cycle assessments (LCA), focussing on solvents like amine and ammonia, are also explored, with summarised information presented in tables for each aspect of the study. It's essential to highlight the significance of conducting studies on the absorption-desorption cycles for several reasons. Firstly, these studies enable the investigation of amine degradation and the reclaiming of amines, shedding light on crucial aspects of solvent performance. Additionally, absorption-desorption cycle studies provide valuable insights into the energy requirements for solvent regeneration. Ultimately, these studies are crucial in the advancement of more stable solvents, offering the potential to reduce the cost associated with solvent-based carbon capture technologies. This approach optimises important performance metrics such as cyclic capacity, recovery quality, and the purity of the treated stream which are critical parameters for CO2 absorption-desorption process.
为了控制全球变暖和大气中的二氧化碳排放,从碳生产源头捕获碳被认为是短期到中期的解决方案。二氧化碳吸收-解吸工艺是公认的成熟工艺,已实施多年。然而,这种工艺有几个弱点,例如解吸装置再生需要大量能源,使用胺溶液时溶剂会降解。在本研究中,我们对二氧化碳捕集的吸收-解吸循环的几个要素进行了研究。其中包括建模、按所采用的单元操作分类的实验、技术经济分析、优化、控制策略和生命周期评估。报告讨论了基于稳态、动态和数据驱动的模型,以及在实验室规模下进行的实验研究,详细介绍了所用溶剂、塔的特性和设备规格。此外,报告还研究了优化技术、技术经济评估(TEA)和工业应用,将其分为电力部门和工业部门,并比较了碳捕集过程的成本和能源需求。此外,还对吸收-解吸系统的不同控制策略进行了回顾、比较和讨论。此外,还探讨了以胺和氨等溶剂为重点的生命周期评估(LCA),并以表格形式汇总了各方面的研究信息。有必要强调对吸收-解吸循环进行研究的重要性,原因有以下几点。首先,通过这些研究可以对胺降解和胺回收进行调查,从而揭示溶剂性能的关键方面。此外,吸收-解吸循环研究为了解溶剂再生所需的能量提供了宝贵的信息。最终,这些研究对于开发更稳定的溶剂至关重要,从而有可能降低基于溶剂的碳捕获技术的相关成本。这种方法可以优化重要的性能指标,如循环能力、回收质量和处理流的纯度,这些都是二氧化碳吸收-解吸过程的关键参数。
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引用次数: 0
Synthesis of nitrogen-doped mesoporous carbon nanospheres using urea-phenol-formaldehyde resin for efficient CO2 adsorption–desorption studies 利用脲-苯酚-甲醛树脂合成氮掺杂介孔碳纳米球,用于高效 CO2 吸附-解吸研究
Pub Date : 2024-10-30 DOI: 10.1016/j.ccst.2024.100302
Rasmeet Singh , Lizhuo Wang , Junhan Cheng , Haoyue Sun , Chunfei Wu , Jun Huang
Global warming led by excessive CO2 emission is a significant challenge. CO2 capture is recognised as an efficient way to mitigate this issue. In this study, we successfully synthesized a series of activation-free nitrogen-doped mesoporous carbon nanospheres (Mx: where x is ratio of urea/phenol) via an aqueous synthesis route, using urea-phenol-formaldehyde resin as a precursor and triblock copolymer F127 as a soft template. These Mx exhibited nitrogen contents ranging from 0.48 % to 1.52 % and with high surface areas within the range of 486.382 to 683.891 m²g⁻¹. Furthermore, they demonstrated a uniform pore channel diameter of around 3.2 nm. The incorporated nitrogen atoms primarily in the forms of pyrrolic, pyridine, and amine groups, offers abundant adsorption sites for CO2. The CO2 adsorption and desorption performance of as-synthesized Mx were systematically studied under various CO2 feed concentrations, including 10 % CO2 by volume, compressed air (mimicking direct air capture (DAC)), and 10 % CO2 by volume at 90 % relative humidity, all at 298 K and ∼1 atm. Interestingly, the M0.1 sample displayed exceptional CO2 capture performance, achieving a capacity of 2.53 mmol g⁻¹ (or 4.8 mmol m⁻²) at a 10 % CO2 by volume feed. This outstanding CO2 adsorption capacity can be attributed to the synergistic effects of ordered mesopore channels, abundant structural micropores, and nitrogen functionalities, facilitating efficient CO2 adsorption and desorption. Additionally, M0.1 also displayed high hydrophobicity character, making it ideal for CO2 adsorption under humid conditions. Moreover, the Mx displayed remarkable stability and recyclability, positioning them as promising and environmentally friendly adsorbents for CO2 capture and separation under practical operating conditions. Additionally, the proposed Mx does not need any additional alkali activation before application, thus simplifying the implementation process, reducing costs, and complexity.
二氧化碳的过度排放导致全球变暖,这是一个重大挑战。二氧化碳捕集被认为是缓解这一问题的有效途径。在这项研究中,我们以尿素-苯酚-甲醛树脂为前驱体,以三嵌段共聚物 F127 为软模板,通过水合成路线成功合成了一系列无活化掺氮介孔碳纳米球(Mx:x 为尿素/苯酚的比例)。这些 Mx 的含氮量在 0.48 % 至 1.52 % 之间,具有 486.382 至 683.891 m²g-¹ 的高表面积。此外,它们还具有约 3.2 纳米的均匀孔道直径。主要以吡咯、吡啶和胺基团形式结合的氮原子为二氧化碳提供了丰富的吸附位点。在 298 K 和 ∼1 atm 条件下,系统地研究了合成的 Mx 在不同二氧化碳进料浓度下的二氧化碳吸附和解吸性能,包括 10% 的二氧化碳(体积比)、压缩空气(模拟直接空气捕获 (DAC))和相对湿度为 90% 的 10% 二氧化碳(体积比)。有趣的是,M0.1 样品显示出卓越的二氧化碳捕获性能,在 10% CO2(体积分数)进料条件下,吸附能力达到 2.53 mmol g-¹(或 4.8 mmol m-²)。这种出色的二氧化碳吸附能力归功于有序的中孔通道、丰富的微孔结构和氮功能的协同作用,从而促进了二氧化碳的高效吸附和解吸。此外,M0.1 还具有较高的疏水性,因此非常适合在潮湿条件下吸附二氧化碳。此外,Mx 还显示出卓越的稳定性和可回收性,使其成为在实际操作条件下捕获和分离二氧化碳的理想环保型吸附剂。此外,拟议的 Mx 在应用前不需要任何额外的碱活化,从而简化了实施过程,降低了成本和复杂性。
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引用次数: 0
Assessment of the volatility of amine degradation compounds in aqueous MEA and blend of 1-(2HE)PRLD and 3A1P 评估水性 MEA 和 1-(2HE)PRLD 与 3A1P 混合液中胺降解化合物的挥发性
Pub Date : 2024-10-30 DOI: 10.1016/j.ccst.2024.100326
Maxime H.J.-J. François , Vanja Buvik , Kai Vernstad , Hanna K. Knuutila
Amine-based carbon capture has proven to be a mature technology, but challenges remain. Emission control of potentially hazardous compounds is critical to ensure the long-term viability of the technology. The ability to predict which compounds to expect in gas emissions and at what levels is fundamental. This work aims to provide a qualitative and quantitative assessment of the volatility of both MEA and HS3 blend degradation products. VLE experiments were performed with different degraded solutions over a temperature range from 40 to 100 °C. Samples were analyzed using extensive LC-MS methods to quantify over 40 degradation compounds. Henry's constants were calculated to assess their volatility. The compiled results allow the ranking of most of the compounds studied in terms of volatility, and the quantification of their relative volatility compared to each other. Pyrazines and alkylamines are among the most volatile, followed by aldehydes, ketones, nitrosamines, and finally, larger amides. When compared, the volatilities of the degradation compounds are consistent from one degraded solution to another, highlighting the possibility of generalization from one solvent to another. This consistency is also observed with the dilute version of the degraded solutions simulating water-wash conditions. Finally, this work provides insight into the temperature dependence of the volatilities of the compounds studied. The methodology used provides a valuable and new type of data that have never been published before on the volatility of amine degradation compounds. The results can be used to better understand emissions and the design of emission control technologies.
胺基碳捕集已被证明是一项成熟的技术,但挑战依然存在。潜在危险化合物的排放控制对于确保该技术的长期可行性至关重要。预测气体排放中会出现哪些化合物以及其含量的能力至关重要。这项工作旨在对 MEA 和 HS3 混合降解产物的挥发性进行定性和定量评估。在 40 至 100 °C 的温度范围内,对不同的降解溶液进行了 VLE 实验。使用广泛的 LC-MS 方法对样品进行分析,以量化 40 多种降解化合物。通过计算亨利常数来评估它们的挥发性。根据汇总的结果,可以对所研究的大部分化合物的挥发性进行排序,并量化它们之间的相对挥发性。吡嗪和烷基胺的挥发性最强,其次是醛、酮、亚硝胺,最后是较大的酰胺。经过比较,不同降解溶液中降解化合物的挥发性是一致的,这说明从一种溶剂到另一种溶剂可以通用。在模拟水洗条件的稀释降解溶液中也观察到了这种一致性。最后,这项研究还深入探讨了所研究化合物的挥发性与温度的关系。所使用的方法提供了有关胺降解化合物挥发性的有价值的新型数据,这些数据以前从未发表过。研究结果可用于更好地了解排放和排放控制技术的设计。
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引用次数: 0
Towards planetary boundary sustainability of food processing wastewater, by resource recovery & emission reduction: A process system engineering perspective 通过资源回收和减排,实现食品加工废水的地球边界可持续性:工艺系统工程视角
Pub Date : 2024-10-30 DOI: 10.1016/j.ccst.2024.100319
Alex Durkin , Tom Vinestock , Miao Guo
Meeting the needs of a growing population calls for a change from linear production systems that exacerbate the depletion of finite natural resources and the emission of environmental pollutants. These linear production systems have resulted in the human-driven perturbation of the Earth’s natural biogeochemical cycles and the transgression of environmentally safe operating limits. One solution that can help alleviate the environmental issues associated both with resource stress and harmful emissions is resource recovery from waste. In this review, we address the recovery of resources from food and beverage processing wastewater (FPWW), which offers a synergistic solution to some of the environmental issues with traditional food production. Research on resource recovery from FPWW typically focuses on technologies to recover specific resources without considering integrative process systems to recover multiple resources while simultaneously satisfying regulations on final effluent quality. Process Systems Engineering (PSE) offers methodologies able to address this holistic process design problem, including modelling the trade-offs between competing objectives. Optimisation of FPWW treatment and resource recovery has significant scope to reduce the environmental impacts of food production systems. There is significant potential to recover carbon, nitrogen, and phosphorus resources while respecting effluent quality limits, even when the significant uncertainties inherent to wastewater systems are considered. This review article gives an overview of the environmental challenges we face, discussed within the framework of the planetary boundary, and highlights the impacts caused by the agri-food sector. This paper also presents a comprehensive review of the characteristics of FPWW and available technologies to recover carbon and nutrient resources from wastewater streams with a particular focus on bioprocesses. PSE research and modelling advances are discussed in this review. Based on this discussion, we conclude the article with future research directions.
要满足日益增长的人口需求,就必须改变加剧有限自然资源耗竭和环境污染排放的线性生产系统。这些线性生产系统导致地球的自然生物地球化学循环受到人为干扰,并突破了环境安全运行极限。从废弃物中回收资源是一个有助于缓解与资源紧张和有害排放相关的环境问题的解决方案。在本综述中,我们将讨论从食品和饮料加工废水(FPWW)中回收资源的问题,这为解决传统食品生产中的一些环境问题提供了一种协同解决方案。从食品饮料加工废水中回收资源的研究通常侧重于回收特定资源的技术,而没有考虑在满足最终出水水质要求的同时回收多种资源的综合工艺系统。工艺系统工程(PSE)提供了能够解决这一整体工艺设计问题的方法,包括对相互竞争的目标之间的权衡进行建模。FPWW 处理和资源回收的优化在减少食品生产系统对环境的影响方面具有重大意义。即使考虑到废水系统固有的重大不确定性,在遵守出水水质限值的同时回收碳、氮和磷资源的潜力也很大。这篇综述文章概述了我们所面临的环境挑战,在地球边界框架内进行了讨论,并强调了农业食品行业所造成的影响。本文还全面回顾了 FPWW 的特点以及从废水流中回收碳和养分资源的现有技术,尤其侧重于生物工艺。本综述还讨论了 PSE 研究和建模方面的进展。在讨论的基础上,我们以未来的研究方向作为文章的结尾。
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引用次数: 0
Exploiting process thermodynamics in carbon capture from direct air to industrial sources: The paradigmatic case of ionic liquids 在从直接空气到工业源的碳捕集过程中利用过程热力学:离子液体的典型案例
Pub Date : 2024-10-30 DOI: 10.1016/j.ccst.2024.100320
Sergio Dorado-Alfaro , Daniel Hospital-Benito , Cristian Moya , Pablo Navarro , Jesús Lemus , José Palomar
<div><div>The development of efficient and cost-effective carbon capture (CC) technologies is becoming a crucial challenge for short-term industrial decarbonization strategies and energy transition goals centred on biomethane and biohydrogen production. Nowadays, available CC technologies present main shortcomings for being applied to the huge wide range of CO<sub>2</sub> partial pressure involved in currently-of-interest industrial CC scenarios (from 0.0004 bar in direct air capture to 13 bar in pre-combustion system: it means five orders of magnitude). Aprotic N-heterocyclic anion-based ionic liquids (AHA-ILs) arise as highly versatile CO<sub>2</sub> chemical absorbents able to deal with this challenge. In this work, the process thermodynamic limits of the CC based on AHA-IL is explored by estimating the thermodynamic CO<sub>2</sub> absorption cyclic capacity (<span><math><msub><mi>z</mi><mrow><mi>c</mi><mi>y</mi><mi>c</mi><mi>l</mi><mi>i</mi><mi>c</mi></mrow></msub></math></span>) for four relevant CC industrial systems [inlet CO<sub>2</sub> partial pressure typical of direct air capture (DAC), post-combustion (post-comb), biogas upgrading (biogas) and pre-combustion (pre-comb)], by means of sensitivity analysis in the literature reported range of key material properties (reaction enthalpy, <span><math><mrow><mstyle><mi>Δ</mi></mstyle><msub><mi>H</mi><mi>R</mi></msub></mrow></math></span>: [−15, −100 kJ/mol]; reaction entropy, <span><math><mrow><mstyle><mi>Δ</mi></mstyle><msub><mi>S</mi><mi>R</mi></msub></mrow></math></span>: [−0.05, −0.16 kJ/mol⋅K]; Henry constant, <span><math><msub><mi>K</mi><mi>H</mi></msub></math></span>: [20, 115 bar]) and process operating conditions (absorption temperature, <span><math><msup><mrow><mi>T</mi></mrow><mrow><mi>a</mi><mi>b</mi><mi>s</mi></mrow></msup></math></span>: [20, 100 °C]; regeneration temperature, <span><math><msup><mrow><mi>T</mi></mrow><mrow><mi>r</mi><mi>e</mi><mi>g</mi></mrow></msup></math></span>: [20, 100 °C]; regeneration pressure, <span><math><msubsup><mi>P</mi><mrow><mi>C</mi><mi>O</mi><mn>2</mn></mrow><mrow><mi>r</mi><mi>e</mi><mi>g</mi></mrow></msubsup></math></span>: [0.01, 0.5 bar]). It is obtained that <span><math><msub><mi>z</mi><mrow><mi>c</mi><mi>y</mi><mi>c</mi><mi>l</mi><mi>i</mi><mi>c</mi></mrow></msub></math></span> can be significantly increased by designing AHA-ILs with more negative <span><math><mrow><mstyle><mi>Δ</mi></mstyle><msub><mi>H</mi><mi>R</mi></msub></mrow></math></span> and <span><math><mrow><mstyle><mi>Δ</mi></mstyle><msub><mi>S</mi><mi>R</mi></msub></mrow></math></span> values, since reaction exothermicity enhances the absorption stage, whereas unfavourable reaction entropy promotes absorbent regeneration. Physical absorption contribution described by <span><math><msub><mi>K</mi><mi>H</mi></msub></math></span> plays a minor role in post-comb and biogas CC systems and becomes highly relevant for pre-comb conditions; surprisingly, DAC process can be enhanced by dec
对于以生物甲烷和生物氢生产为核心的短期工业脱碳战略和能源转型目标而言,开发高效且具有成本效益的碳捕集(CC)技术正成为一项重要挑战。目前,现有的碳捕集(CC)技术在应用于目前感兴趣的工业碳捕集(CC)方案所涉及的巨大二氧化碳分压范围(从直接空气捕集的 0.0004 巴到预燃烧系统的 13 巴:这意味着五个数量级)方面存在主要缺陷。Aprotic N-heterocyclic 阴离子基离子液体(AHA-ILs)作为高度通用的二氧化碳化学吸收剂,能够应对这一挑战。在这项工作中,通过对文献报道的关键材料属性范围(反应焓,ΔHR.[-15, -100 kJ])进行敏感性分析,估算了四种相关 CC 工业系统[典型的直接空气捕集(DAC)、燃烧后(post-comb)、沼气升级(biogas)和燃烧前(pre-comb)的入口二氧化碳分压]的热力学二氧化碳吸收循环能力(zcyclic),从而探索了基于 AHA-IL 的 CC 的工艺热力学极限:[-15,-100 kJ/mol];反应熵,ΔSR:[-0.05,-0.16 kJ/mol-K];亨利常数,KH:[20,115 bar])和工艺操作条件(吸收温度,Tabs:[20,100 °C]; 再生温度,Treg:[20,100 °C]; 再生压力,PCO2reg:[0.01,0.5 bar])。结果表明,通过设计具有更多负值 ΔHR 和 ΔSR 的 AHA-IL 可以显著提高 zcyclic 值,因为反应放热会增强吸收阶段,而不利的反应熵则会促进吸收剂的再生。KH 所描述的物理吸收作用在后化学反应和沼气 CC 系统中作用较小,而在前化学反应条件下则变得非常重要;令人惊讶的是,DAC 过程可以通过降低材料的 KH 值来增强。至于工艺操作条件的影响,通过降低 Tabs 和 PCO2reg 以及增加 Treg 可以提高 CC 循环能力,但不同 CC 方案的影响明显不同:在预混合系统中,z 循环几乎不受影响,而在 DAC 中,工艺条件是获得正 z 循环值的决定因素。最后,对现有文献中的ΔHR、ΔSR 和 KH 的批判性分析表明,通过微调阳离子和阴离子结构来设计 AHA-IL 材料,非常适合于开发具有更佳 CC 工艺性能的创新技术,尤其适用于更具挑战性的 DAC 和稀释碳源捕获。
{"title":"Exploiting process thermodynamics in carbon capture from direct air to industrial sources: The paradigmatic case of ionic liquids","authors":"Sergio Dorado-Alfaro ,&nbsp;Daniel Hospital-Benito ,&nbsp;Cristian Moya ,&nbsp;Pablo Navarro ,&nbsp;Jesús Lemus ,&nbsp;José Palomar","doi":"10.1016/j.ccst.2024.100320","DOIUrl":"10.1016/j.ccst.2024.100320","url":null,"abstract":"&lt;div&gt;&lt;div&gt;The development of efficient and cost-effective carbon capture (CC) technologies is becoming a crucial challenge for short-term industrial decarbonization strategies and energy transition goals centred on biomethane and biohydrogen production. Nowadays, available CC technologies present main shortcomings for being applied to the huge wide range of CO&lt;sub&gt;2&lt;/sub&gt; partial pressure involved in currently-of-interest industrial CC scenarios (from 0.0004 bar in direct air capture to 13 bar in pre-combustion system: it means five orders of magnitude). Aprotic N-heterocyclic anion-based ionic liquids (AHA-ILs) arise as highly versatile CO&lt;sub&gt;2&lt;/sub&gt; chemical absorbents able to deal with this challenge. In this work, the process thermodynamic limits of the CC based on AHA-IL is explored by estimating the thermodynamic CO&lt;sub&gt;2&lt;/sub&gt; absorption cyclic capacity (&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mi&gt;z&lt;/mi&gt;&lt;mrow&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mi&gt;y&lt;/mi&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mi&gt;l&lt;/mi&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;) for four relevant CC industrial systems [inlet CO&lt;sub&gt;2&lt;/sub&gt; partial pressure typical of direct air capture (DAC), post-combustion (post-comb), biogas upgrading (biogas) and pre-combustion (pre-comb)], by means of sensitivity analysis in the literature reported range of key material properties (reaction enthalpy, &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mstyle&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mstyle&gt;&lt;msub&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;mi&gt;R&lt;/mi&gt;&lt;/msub&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;: [−15, −100 kJ/mol]; reaction entropy, &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mstyle&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mstyle&gt;&lt;msub&gt;&lt;mi&gt;S&lt;/mi&gt;&lt;mi&gt;R&lt;/mi&gt;&lt;/msub&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;: [−0.05, −0.16 kJ/mol⋅K]; Henry constant, &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mi&gt;K&lt;/mi&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;: [20, 115 bar]) and process operating conditions (absorption temperature, &lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;a&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;mi&gt;s&lt;/mi&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt;: [20, 100 °C]; regeneration temperature, &lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;r&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;mi&gt;g&lt;/mi&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt;: [20, 100 °C]; regeneration pressure, &lt;span&gt;&lt;math&gt;&lt;msubsup&gt;&lt;mi&gt;P&lt;/mi&gt;&lt;mrow&gt;&lt;mi&gt;C&lt;/mi&gt;&lt;mi&gt;O&lt;/mi&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;r&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;mi&gt;g&lt;/mi&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;/math&gt;&lt;/span&gt;: [0.01, 0.5 bar]). It is obtained that &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mi&gt;z&lt;/mi&gt;&lt;mrow&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mi&gt;y&lt;/mi&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;mi&gt;l&lt;/mi&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;mi&gt;c&lt;/mi&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; can be significantly increased by designing AHA-ILs with more negative &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mstyle&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mstyle&gt;&lt;msub&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;mi&gt;R&lt;/mi&gt;&lt;/msub&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; and &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mstyle&gt;&lt;mi&gt;Δ&lt;/mi&gt;&lt;/mstyle&gt;&lt;msub&gt;&lt;mi&gt;S&lt;/mi&gt;&lt;mi&gt;R&lt;/mi&gt;&lt;/msub&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; values, since reaction exothermicity enhances the absorption stage, whereas unfavourable reaction entropy promotes absorbent regeneration. Physical absorption contribution described by &lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mi&gt;K&lt;/mi&gt;&lt;mi&gt;H&lt;/mi&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; plays a minor role in post-comb and biogas CC systems and becomes highly relevant for pre-comb conditions; surprisingly, DAC process can be enhanced by dec","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"13 ","pages":"Article 100320"},"PeriodicalIF":0.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551548","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Recent advances in H2 purification and CO2 capture: Evolving from flat sheet to hollow fiber membranes H2 净化和 CO2 捕获的最新进展:从平板膜到中空纤维膜的演变
Pub Date : 2024-10-29 DOI: 10.1016/j.ccst.2024.100334
Jun Yi Teh , Wai Fen Yong
Hydrogen (H2) production and demand have steadily increased, leading to a rise in carbon dioxide (CO2) emissions since fossil fuels are the current raw material for H2 production. Thin film composite (TFC) hollow fiber membranes have become significant in H2 purification and CO2 capture, playing a critical role in developing next-generation fuels and supporting the United Nations Sustainable Development Goal 7 (SDG 7) – Affordable and Clean Energy, with the goal of providing universal access to clean, advanced, and renewable energy for all. However, the polymeric selective layer of TFC membranes faces a trade-off between permeability and selectivity, as well as challenges including CO2 plasticization and physical aging. Additionally, H2/CO2 separation remains particularly challenging because H2, being diffusivity-selective, permeates more quickly through the membrane due to its smaller molecular size and higher kinetic energy, while CO2, being solubility-selective, has a high affinity for dissolving in most polymeric membranes. Herein, this review provides an in-depth exploration of innovative modification strategies designed to overcome these challenges in glassy polymeric membranes and enhance H2 separation performance in the recent 10 years. Various nanofillers, such as metal-organic frameworks (MOFs) such as University of Oslo (UiO), Materials Institute Lavoisier (MILs), and Zeolitic Imidazolate Frameworks (ZIFs), have shown remarkable potential in boosting gas separation capabilities due to their superior compatibility with polymer matrices and tunable properties. The review also explores different types of hollow fiber membranes, including single layer, dual-layer, and TFC, alongside fabrication techniques like interfacial polymerization and dip-coating. Critically, the analysis highlights cutting-edge strategies to improve membrane performance, such as (i) thermal cross-linking, (ii) chemical cross-linking, (iii) ultraviolet (UV) cross-linking, (iv) polymer blends, and (v) modified fillers, along with their objectives and expected outcome. Furthermore, the review spotlights breakthroughs in H2/CO2, H2/CH4, and H2/N2 separation technologies, emphasizing the critical need for continued innovation to drive sustainable H2 production and meet the growing clean energy demand.
氢气(H2)的生产和需求稳步增长,导致二氧化碳(CO2)排放量增加,因为化石燃料是目前生产 H2 的原材料。薄膜复合(TFC)中空纤维膜在 H2 净化和二氧化碳捕获方面具有重要作用,在开发下一代燃料和支持联合国可持续发展目标 7(SDG 7)--负担得起的清洁能源方面发挥着至关重要的作用,该目标旨在为所有人普及清洁、先进和可再生能源。然而,TFC 膜的聚合物选择层面临着渗透性和选择性之间的权衡,以及二氧化碳塑化和物理老化等挑战。此外,H2/CO2 分离仍然特别具有挑战性,因为具有扩散选择性的 H2 因其分子尺寸较小和动能较高而更快地透过膜,而具有溶解选择性的 CO2 在大多数聚合物膜中具有较高的溶解亲和力。在此,本综述深入探讨了近 10 年来旨在克服玻璃聚合物膜中的这些挑战并提高 H2 分离性能的创新改性策略。各种纳米填料,如奥斯陆大学(UiO)、拉瓦锡材料研究所(MILs)和沸石咪唑框架(ZIFs)等金属有机框架(MOFs),因其与聚合物基质的卓越兼容性和可调特性,在提高气体分离能力方面已显示出显著的潜力。综述还探讨了不同类型的中空纤维膜,包括单层膜、双层膜和 TFC 膜,以及界面聚合和浸涂等制造技术。重要的是,分析强调了提高膜性能的前沿策略,如(i)热交联、(ii)化学交联、(iii)紫外线(UV)交联、(iv)聚合物混合物和(v)改性填料,以及它们的目标和预期结果。此外,综述还重点介绍了在 H2/CO2、H2/CH4 和 H2/N2 分离技术方面取得的突破,强调了持续创新以推动可持续 H2 生产和满足日益增长的清洁能源需求的迫切需要。
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引用次数: 0
Hydrothermal reduction of CO2 captured by aqueous amine solutions into formate: Comparison between in situ generated H2 and gaseous H2 as reductant and evaluation of amine stability 胺水溶液将捕获的 CO2 水热还原为甲酸盐:比较原位生成的 H2 与作为还原剂的气态 H2,评估胺的稳定性
Pub Date : 2024-10-28 DOI: 10.1016/j.ccst.2024.100333
Laura Quintana-Gómez , Luana Cristina Dos Santos , Fernando Cossio-Cid , Víctor Ciordia-Asenjo , Miguel Almarza , Alberto Goikoechea , Sergio Ferrero , Celedonio M․ Álvarez , José J․ Segovia , Ángel Martín , M․Dolores Bermejo
By CO2 Capture and Utilization technologies (CCU), organic compounds can be produced industrially in a sustainable manner, generating an economic benefit that offsets the cost of CO2 capture. In this context, the use of CO2 chemisorbed by amines to generate chemicals is an attractive alternative, given that large-scale facilities using absorption to capture CO2 are already operational. The aim of this work is to convert CO2 captured in aqueous amines, specifically 3-amino-1-propanol (AP) and 2-amino-2-methyl-1-propanol (AMP), to produce formate, using either Zn, Al or gaseous H2 as reductants and Pd/C as catalyst. The highest yield of formate (68 %) was achieved with AP (125 °C, 75 bar, 120 min) using gaseous hydrogen as reductant. Using metals as reductants, reaction yields were lower, with a 12 % yield at 200 °C as the best result. After reduction, NMR analyses show that the amines did not suffer degradation, raising the possibility of reusing them for CO2 capture in a continuous process. These results indicate that CO2-loaded amines reduction is a promising CCU technology that can be integrated with the current technologies for gas treatment.
通过二氧化碳捕获和利用技术(CCU),可以以可持续的方式在工业上生产有机化合物,产生的经济效益可以抵消二氧化碳捕获的成本。在这种情况下,利用胺对二氧化碳进行化学吸附来生产化学品是一种有吸引力的替代方法,因为利用吸收技术捕获二氧化碳的大型设施已经投入使用。这项工作的目的是利用 Zn、Al 或气态 H2 作为还原剂,Pd/C 作为催化剂,将捕集到水胺(特别是 3-氨基-1-丙醇 (AP) 和 2-氨基-2-甲基-1-丙醇 (AMP))中的二氧化碳转化为甲酸盐。使用气态氢作为还原剂,在 AP(125 °C,75 巴,120 分钟)条件下甲酸盐的产量最高(68%)。使用金属作为还原剂时,反应产率较低,200 ℃ 时的最佳产率为 12%。还原后的核磁共振分析表明,胺类物质没有发生降解,因此有可能在连续工艺中将其重新用于二氧化碳捕获。这些结果表明,二氧化碳负载胺还原是一种很有前景的 CCU 技术,可以与当前的气体处理技术相结合。
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引用次数: 0
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Carbon Capture Science & Technology
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