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The advancements in mixed matrix membranes containing functionalized MOFs and 2D materials for CO2/N2 separation and CO2/CH4 separation 含有功能化 MOF 和二维材料的混合基质膜在 CO2/N2 分离和 CO2/CH4 分离方面取得的进展
Pub Date : 2024-08-08 DOI: 10.1016/j.ccst.2024.100267

CO2 separation plays a crucial role in tackling the climate change induced by the greenhouse effects and improving the energy quality of natural gas and biogas. The efficient CO2 separation technology is highly required. Membrane separation technology is particularly attractive in CO2 separation processes owing to its advantages. However, the trade-off relationship limited the gas separation efficiency of polymeric membranes in gas separation processes. Therefore, it is necessary to prepare the high-performance membranes such as mixed matrix membranes (MMMs) for CO2 separation. This review mainly focuses on the preparation methods, the material properties and the CO2 separation efficiency of the MMMs containing various fillers such as modified ZIFs, MOFs, and GO, and the emerging MOF-based composites, 2D MOFs and 2D MXene. The modified fillers demonstrated higher compatibility with polymer matrix, resulting in enhanced mechanical stability and CO2 separation efficiency of MMMs. 2D materials could significantly enhance the CO2 separation efficiency of MMMs, owing to their layered structure and the effective regulation of gas transport ways. Finally, the future direction and conclusions of fillers and MMMs in gas separation processes are provided.

二氧化碳分离在应对温室效应引起的气候变化以及提高天然气和沼气的能源质量方面发挥着至关重要的作用。高效的二氧化碳分离技术非常必要。膜分离技术因其优势在二氧化碳分离过程中尤其具有吸引力。然而,权衡关系限制了聚合物膜在气体分离过程中的气体分离效率。因此,有必要制备用于二氧化碳分离的高性能膜,如混合基质膜(MMMs)。本综述主要关注含有各种填料(如改性 ZIF、MOF 和 GO)的 MMMs 以及新兴的基于 MOF 的复合材料、二维 MOF 和二维 MXene 的制备方法、材料性能和二氧化碳分离效率。改性填料与聚合物基体具有更高的相容性,从而提高了 MMM 的机械稳定性和二氧化碳分离效率。二维材料由于其层状结构和对气体传输途径的有效调节,可大大提高 MMMs 的二氧化碳分离效率。最后,介绍了填料和 MMMs 在气体分离过程中的未来发展方向和结论。
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引用次数: 0
Near-equilibrium analysis of CO2 partial pressure on carbonate hydrogenation in an integrated carbon capture and utilization scheme 二氧化碳分压对碳捕获和利用综合方案中碳酸盐加氢的近平衡分析
Pub Date : 2024-08-08 DOI: 10.1016/j.ccst.2024.100261

The integrated carbon capture and utilization (ICCU) technology, combined with the reverse water-gas shift reaction (RWGS), is considered a promising strategy for mitigating carbon emissions. This study investigates the limestone calcination and hydrogenation processes under relatively high partial pressures of CO2 in near-equilibrium conditions, at partial pressures (P) close to the equilibrium pressure (Peq), relevant to the ICCU-RWGS process, particularly during the in-situ CO2 conversion stage. The decomposition of CaCO3 during conventional calcination and hydrogenation under near-equilibrium conditions was initially examined using micro-fluidized bed thermogravimetric analysis coupled with mass spectrometry (MFB-TGA-MS) and a particle-injecting method. The results indicated that limestone decomposition during conventional calcination was inhibited under near-equilibrium conditions, with conversion near 0%. However, during the hydrogenation process, the interaction between H2 and CaCO3 further activated the decomposition of limestone. At 750 °C and P/Peq=0.9, limestone particles took ∼100 s to achieve complete conversion (100%). Given the known self-catalytic activity of CaO in converting carbonate to CO during hydrogenation, a dual-layer limestone hydrogenation process was further conducted using a fixed bed reactor. At 850 °C and a 30 vol.% H2 atmosphere, the limestone decomposition rate increased significantly and subsequently reacted with H2 to form CO, resulting in an H2/CO ratio of approximately 2.5. These findings support the viability of ICCU-RWGS approaches for future commercialization, with the product gas serving as the feedstock for the Fischer–Tropsch Synthesis (FTS) process.

综合碳捕集与利用(ICCU)技术与反向水气变换反应(RWGS)相结合,被认为是一种很有前途的减少碳排放的策略。本研究对石灰石煅烧和氢化过程进行了研究,在接近平衡条件下,在接近平衡压力(Peq)的分压(P)下,特别是在二氧化碳原位转化阶段,石灰石煅烧和氢化过程与 ICCU-RWGS 过程相关。利用微流化床热重分析与质谱联用技术(MFB-TGA-MS)和颗粒注入法对近平衡条件下传统煅烧和加氢过程中 CaCO3 的分解进行了初步研究。结果表明,在接近平衡的条件下,石灰石在传统煅烧过程中的分解受到抑制,转化率接近 0%。然而,在氢化过程中,H2 和 CaCO3 之间的相互作用进一步激活了石灰石的分解。在 750 °C 和 P/Peq=0.9 的条件下,石灰石颗粒需要 100 秒才能实现完全转化(100%)。鉴于已知 CaO 在氢化过程中将碳酸盐转化为 CO 的自催化活性,我们使用固定床反应器进一步进行了双层石灰石氢化过程。在 850 °C 和 30 Vol.% H2 的气氛下,石灰石的分解率显著增加,随后与 H2 反应生成 CO,从而使 H2/CO 比率达到约 2.5。这些发现证明了 ICCU-RWGS 方法在未来商业化的可行性,其产品气体可作为费托合成(FTS)工艺的原料。
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引用次数: 0
Comparative review of biodiesel production and purification 生物柴油生产和提纯比较综述
Pub Date : 2024-08-08 DOI: 10.1016/j.ccst.2024.100264

Biodiesel synthesis and purification are critical stages in the production process, continually evolving to address environmental concerns and improve operational efficiency. Currently, biodiesel production has seen significant growth with numerous commercial plants operating worldwide, contributing to the blend of biodiesel with fossil fuels to reduce carbon emissions. Diverse feedstocks, including vegetable oils, animal fats, and waste oils, are increasingly used to enhance the sustainability of biodiesel production. This review examines recent innovations and challenges in biodiesel synthesis and purification, encompassing a diverse range of methodologies. Emphasizing the importance of biodiesel feedstock, the study conducts a comprehensive analysis of various sources contributing to biodiesel production. Synthesis methods, including transesterification, direct use, blending, micro-emulsion, and thermal cracking, are evaluated for their environmental impact and economic feasibility. Furthermore, purification strategies such as wet washing, distillation, adsorption, membrane separation, and solvent-aided crystallization (SAC) are scrutinized for their effectiveness and environmental implications. The review discusses the role of technological advancements in addressing challenges associated with traditional methods, such as high water consumption, energy-intensive processes, and wastewater generation. Moreover, it provides insights into how these innovations can enhance the sustainability, cost-effectiveness, and scalability of biodiesel production. This academically rigorous review offers a nuanced understanding of biodiesel production, combining analysis of feedstock considerations, synthesis methods, and purification strategies to advance discourse on sustainable biofuel production.

生物柴油的合成和提纯是生产过程中的关键阶段,不断发展以解决环境问题并提高运营效率。目前,生物柴油生产有了显著增长,全球有许多商业工厂在运营,这有助于生物柴油与化石燃料的混合,从而减少碳排放。为了提高生物柴油生产的可持续性,包括植物油、动物脂肪和废油在内的多种原料正被越来越多地使用。本综述探讨了生物柴油合成和提纯方面的最新创新和挑战,包括各种不同的方法。本研究强调生物柴油原料的重要性,对生物柴油生产的各种来源进行了全面分析。对包括酯交换、直接使用、混合、微乳化和热裂解在内的合成方法的环境影响和经济可行性进行了评估。此外,还仔细研究了湿洗、蒸馏、吸附、膜分离和溶剂辅助结晶(SAC)等提纯策略的有效性和对环境的影响。综述讨论了技术进步在应对与传统方法相关的挑战(如高耗水量、能源密集型工艺和废水产生)方面的作用。此外,它还深入探讨了这些创新如何提高生物柴油生产的可持续性、成本效益和可扩展性。这篇严谨的学术综述对生物柴油的生产提供了细致入微的理解,结合了对原料考虑因素、合成方法和提纯策略的分析,推动了对可持续生物燃料生产的讨论。
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引用次数: 0
Initial results of a pilot project for sub-seabed basalt storage of carbon dioxide on the Reykjanes Ridge 雷克雅内斯海脊海底玄武岩下封存二氧化碳试点项目的初步成果
Pub Date : 2024-08-08 DOI: 10.1016/j.ccst.2024.100265

To meet temperature goals that limit warming to well below 2 °C requires the removal of hundreds of billions of tonnes of CO2 from the atmosphere over the course of this century. Effective Carbon Dioxide Removal (CDR) methodologies will be required to reduce net emissions in the near term, counterbalance residual CO2 emissions to achieve net-zero in the medium term, and contribute to net-negative emissions in the longer term – all of this in a sustainable and safe manner. This paper summarizes the research objectives and selected initial results of a collaborative project to assess CO2 storage in the upper ocean crust south of Iceland.

The AIMS3 project (www.aims3.cdrmare.de) will deliver new insights, monitoring tools and feasibility assessments for CO2 storage in young, reactive basalts with little sedimentary cover. Along the flank of the Mid-Atlantic Ridge, we have done geophysical surveys and drilled a transect of boreholes in order to identify fluid migration in the upper ocean crust. Both in situ heat flow and geochemical signatures provide irrefutable evidence for such transport, which will help distributing injected CO2 in future experiments.

In parallel, our project also has mineralization experiments to assess optimal conditions for injection dissolved, liquid, or supercritical CO2), numerical modelling for upscaling our results from seagoing work, and development of cost-effective sensors and smart robotic landers for long-term monitoring of the vicinity of the boreholes. We outline the rationale of AIMS3, provide an overview of the activities, and highlight some of the expedition results, with the goal to stimulate communication and collaboration.

要实现将升温控制在远低于 2 °C 的温度目标,就需要在本世纪从大气中清除数千亿吨二氧化碳。有效的二氧化碳清除(CDR)方法需要在短期内减少净排放量,在中期内抵消剩余的二氧化碳排放量以实现净零排放,并在长期内实现净负排放--所有这些都要以可持续和安全的方式进行。本文总结了一个合作项目的研究目标和部分初步成果,该项目旨在评估冰岛南部上层洋壳的二氧化碳封存情况。AIMS3 项目(www.aims3.cdrmare.de)将为在沉积覆盖较少的年轻活性玄武岩中封存二氧化碳提供新的见解、监测工具和可行性评估。沿大西洋中脊侧翼,我们进行了地球物理勘测,并钻探了横断面钻孔,以确定上洋壳中的流体迁移。与此同时,我们的项目还进行了矿化实验,以评估注入溶解、液体或超临界二氧化碳的最佳条件;进行了数值建模,以升级我们的海上工作成果;开发了具有成本效益的传感器和智能机器人着陆器,以对钻孔附近进行长期监测。我们概述了 AIMS3 的基本原理,提供了活动概览,并重点介绍了部分考察成果,旨在促进交流与合作。
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引用次数: 0
Bifunctionality of amine-modified metal-organic frameworks for CO2 capture and selective utilization in cycloaddition 胺修饰金属有机框架在环化反应中捕获和选择性利用二氧化碳的双功能性
Pub Date : 2024-08-03 DOI: 10.1016/j.ccst.2024.100262

In this study, copper- and chromium-based (HKUST-1 and MIL-101(Cr), respectively) metal-organic frameworks (MOF) functionalized with amine groups (HKUST-1‒NH2 and MIL-101(Cr)‒NH2, respectively) were directly synthesized using 2-aminoterephthalic acid as an organic linker via hydrothermal method without adding hydrofluoric acid. They were then investigated for their potential applications in dynamic carbon dioxide (CO2) adsorption and conversion of epoxides with CO2. The functionalized MOF (HKUST-1‒NH2 and MIL-101(Cr)‒NH2) retained their desired textural properties, while gaining a significantly enhanced Lewis basic character for CO2 capture and catalysis application. Both HKUST-1‒NH2 and MIL-101(Cr)‒NH2 not only showed an improved CO2 uptake capability, but also an excellent and stable regenerability over multiple adsorption-desorption cycles. MIL-101(Cr)‒NH2 exhibited a higher performance than the parent MOF and HKUST-1‒NH2 in the transformation of styrene oxide (SO) with CO2 to styrene carbonate (SC) and carbonate oligomers (COL) due to combined effect of its textural properties and basicity. Under solvent-free system, COL from monomeric SC was directly obtained, up to 72.4 % yield, via in situ oligomerization. Optimization of the solvent-free reaction conditions was carried out to control the selective pathway of CO2 utilization between cycloaddition and oligomerization. In the presence of acetonitrile, a > 97 % yield of SC was achieved over MIL-101(Cr)‒NH2 under a mild reaction condition (120 °C and 20 bar of CO2). Reaction mechanisms for the cycloaddition and oligomerization of SO with CO2 are also proposed to comprehend the role of MOF, amine group, and co-catalyst. The combined efficient CO2 adsorption and capability to produce CC and COL makes the synthesized MOF promising materials for CO2 capture and selective utilization.

本研究以 2-aminoterephthalic acid(2-氨基对苯二甲酸)为有机连接体,通过水热法直接合成了含胺基(HKUST-1-NH2 和 MIL-101(Cr)-NH2)的铜基和铬基(分别为 HKUST-1 和 MIL-101(Cr))金属有机框架(MOF),无需添加氢氟酸。然后研究了它们在动态二氧化碳(CO2)吸附和环氧化物与 CO2 转化中的潜在应用。功能化 MOF(HKUST-1-NH2 和 MIL-101(Cr)-NH2)保留了它们所需的纹理特性,同时在二氧化碳捕获和催化应用中获得了显著增强的路易斯碱性。HKUST-1-NH2 和 MIL-101(Cr)-NH2 不仅提高了二氧化碳的吸收能力,而且在多次吸附-解吸循环中都具有出色而稳定的再生能力。与母体 MOF 和 HKUST-1-NH2 相比,MIL-101(Cr)-NH2 在氧化苯乙烯(SO)与 CO2 转化为碳酸苯乙烯(SC)和碳酸苯乙烯低聚物(COL)的过程中表现出更高的性能,这是由其质地特性和碱性共同作用的结果。在无溶剂体系下,通过原位低聚,可直接从单体 SC 中获得 COL,收率高达 72.4%。对无溶剂反应条件进行了优化,以控制二氧化碳在环化和低聚之间的选择性利用途径。在存在乙腈的温和反应条件下(120 °C 和 20 bar CO2),MIL-101(Cr)-NH2 的 SC 收率达到了 97%。此外,还提出了 SO 与 CO2 环加成和低聚的反应机理,以理解 MOF、胺基和助催化剂的作用。所合成的 MOF 既能高效吸附 CO2,又能生成 CC 和 COL,因此是很有前途的 CO2 捕获和选择性利用材料。
{"title":"Bifunctionality of amine-modified metal-organic frameworks for CO2 capture and selective utilization in cycloaddition","authors":"","doi":"10.1016/j.ccst.2024.100262","DOIUrl":"10.1016/j.ccst.2024.100262","url":null,"abstract":"<div><p>In this study, copper- and chromium-based (HKUST-1 and MIL-101(Cr), respectively) metal-organic frameworks (MOF) functionalized with amine groups (HKUST-1‒NH<sub>2</sub> and MIL-101(Cr)‒NH<sub>2</sub>, respectively) were directly synthesized using 2-aminoterephthalic acid as an organic linker via hydrothermal method without adding hydrofluoric acid. They were then investigated for their potential applications in dynamic carbon dioxide (CO<sub>2</sub>) adsorption and conversion of epoxides with CO<sub>2</sub>. The functionalized MOF (HKUST-1‒NH<sub>2</sub> and MIL-101(Cr)‒NH<sub>2</sub>) retained their desired textural properties, while gaining a significantly enhanced Lewis basic character for CO<sub>2</sub> capture and catalysis application. Both HKUST-1‒NH<sub>2</sub> and MIL-101(Cr)‒NH<sub>2</sub> not only showed an improved CO<sub>2</sub> uptake capability, but also an excellent and stable regenerability over multiple adsorption-desorption cycles. MIL-101(Cr)‒NH<sub>2</sub> exhibited a higher performance than the parent MOF and HKUST-1‒NH<sub>2</sub> in the transformation of styrene oxide (SO) with CO<sub>2</sub> to styrene carbonate (SC) and carbonate oligomers (COL) due to combined effect of its textural properties and basicity. Under solvent-free system, COL from monomeric SC was directly obtained, up to 72.4 % yield, via <em>in situ</em> oligomerization. Optimization of the solvent-free reaction conditions was carried out to control the selective pathway of CO<sub>2</sub> utilization between cycloaddition and oligomerization. In the presence of acetonitrile, <em>a</em> &gt; 97 % yield of SC was achieved over MIL-101(Cr)‒NH<sub>2</sub> under a mild reaction condition (120 °C and 20 bar of CO<sub>2</sub>). Reaction mechanisms for the cycloaddition and oligomerization of SO with CO<sub>2</sub> are also proposed to comprehend the role of MOF, amine group, and co-catalyst. The combined efficient CO<sub>2</sub> adsorption and capability to produce CC and COL makes the synthesized MOF promising materials for CO<sub>2</sub> capture and selective utilization.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000745/pdfft?md5=cfddabca0a6d086245424f4d35279d5d&pid=1-s2.0-S2772656824000745-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141961326","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
Synergistic CO2 capture using PANI-polymerized UiO-66 embedded in PEBAX mixed matrix membranes 使用嵌入 PEBAX 混合基质膜的 PANI 聚合 UiO-66 协同捕获二氧化碳
Pub Date : 2024-08-02 DOI: 10.1016/j.ccst.2024.100260

In this study, mixed-matrix membranes (MMMs) were fabricated using a composite of UiO-66 and polyaniline (PANI) integrated into a polyether-block-amide (PEBAX) matrix. The successful synthesis of the UiO-66 and PANI@UiO-66 composites and their incorporation into the PEBAX matrix were validated through X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Fourier Transform Infrared (FTIR) Spectroscopy, Brunauer–Emmett–Teller (BET) analysis, and Thermogravimetric Analysis (TGA). Quantitative permeation tests revealed that the CO2 permeability in UiO-66 based MMMs increased by 90 % at 30 % filler loading (from 82 to 156 Barrer), and by 45 % (from 82 to 119 Barrer) in PANI@UiO-66 based MMMs, alongside substantial improvements in selectivity. For UiO-66 membranes we observed a selectivity drop for both gas pairs (CO2/CH4 and CO2/N2) that led to our motivation to modify the MOF. The CO2/CH4 selectivity of the PANI@UiO-66 based MMMs enhanced from 22 to 29 (34%) and the CO2/N2 selectivity from 48 to 57 (18%). Mixed-gas permeation tests further confirmed the efficacy of the membranes in real-world separation scenarios. The diffusivity and solubility results provide insights into the gas transport mechanisms, revealing the synergistic effects of filler incorporation on membrane performance. The integration of UiO-66 and PANI with PEBAX offers a promising pathway for developing efficient and effective gas separation technologies, aligning with the industrial requirements for environmental sustainability and energy efficiency.

本研究利用 UiO-66 和聚苯胺 (PANI) 的复合材料与聚醚嵌段酰胺 (PEBAX) 基质的结合制造了混合基质膜 (MMM)。通过 X 射线衍射 (XRD)、扫描电子显微镜 (SEM)、傅立叶变换红外光谱 (FTIR)、Brunauer-Emmett-Teller (BET) 分析和热重分析 (TGA),验证了 UiO-66 和 PANI@UiO-66 复合材料的成功合成及其与 PEBAX 基质的结合。定量渗透测试表明,在 UiO-66 基 MMM 中,当填料负载量为 30% 时,二氧化碳渗透率提高了 90%(从 82 巴勒提高到 156 巴勒),而在 PANI@UiO-66 基 MMM 中,二氧化碳渗透率提高了 45%(从 82 巴勒提高到 119 巴勒),同时选择性也大幅提高。对于 UiO-66 膜,我们观察到两种气体对(CO2/CH4 和 CO2/N2)的选择性都有所下降,这促使我们对 MOF 进行改性。基于 PANI@UiO-66 的 MMM 的 CO2/CH4 选择性从 22 提高到 29(34%),CO2/N2 选择性从 48 提高到 57(18%)。混合气体渗透测试进一步证实了膜在实际分离应用中的功效。扩散率和溶解度结果提供了对气体传输机制的深入了解,揭示了填料的加入对膜性能的协同效应。UiO-66 和 PANI 与 PEBAX 的整合为开发高效的气体分离技术提供了一条前景广阔的途径,符合工业对环境可持续性和能源效率的要求。
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引用次数: 0
Potential of carbon dioxide spraying on the properties of 3D concrete printed structures 二氧化碳喷射对三维混凝土打印结构性能的影响
Pub Date : 2024-08-02 DOI: 10.1016/j.ccst.2024.100256

Achieving net carbon neutrality is a global goal toward mitigating climate change presumed consequences. The building and construction sector, responsible for approximately 40 % of greenhouse gas emissions, requires innovative zero-carbon technologies. This paper investigates the synergistic potential of combining 3D concrete printing (3DCP) and carbon capture and sequestration (CCS) to advance net carbon neutrality in construction. By implementing different CO2 spraying regimes, this study demonstrates improved carbon dioxide (CO2) uptake and the crystallinity of precipitated calcium carbonate (CaCO3). The findings indicate that the method's effectiveness heavily relies on appropriate printing parameters and curing conditions. Chamber-cured samples exhibit the highest CO2 uptake but the lowest mechanical strength, while ambient-cured samples show the opposite trend. It is also important to note that the duration of CO2 exposure in this study was relatively short, resulting in limitations in both CO2 uptake and strength gain. Nevertheless, this study highlights the potential of synergistically combining 3DCP and CCS technologies for net carbon neutrality, emphasizing the critical role of the construction sector in achieving global emission reduction targets.

实现净碳中和是减缓气候变化假定后果的全球目标。建筑施工行业约占温室气体排放的 40%,需要创新的零碳技术。本文研究了三维混凝土打印(3DCP)与碳捕集与封存(CCS)的协同潜力,以推进建筑业的净碳中和。通过采用不同的二氧化碳喷洒机制,本研究证明了二氧化碳(CO2)吸收和沉淀碳酸钙(CaCO3)结晶度的改善。研究结果表明,该方法的有效性在很大程度上取决于适当的印刷参数和固化条件。室温固化的样品二氧化碳吸收量最高,但机械强度最低,而常温固化的样品则呈现出相反的趋势。还需要注意的是,本研究中的二氧化碳暴露时间相对较短,导致二氧化碳吸收和强度增加都受到限制。尽管如此,本研究强调了将 3DCP 和 CCS 技术协同结合以实现净碳中和的潜力,强调了建筑行业在实现全球减排目标中的关键作用。
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引用次数: 0
High temperature capture of CO2 on Li4SiO4 sorbents via a simple dry ball-milling coupled with K2CO3 physical addition 通过简单的干法球磨和 K2CO3 物理添加,在 Li4SiO4 吸附剂上实现二氧化碳的高温捕获
Pub Date : 2024-08-01 DOI: 10.1016/j.ccst.2024.100255

The reversible CO2 absorption/desorption of lithium orthosilicate (Li4SiO4) sorbents holds potential for high temperature capture of CO2 from hot flue gases, sorption-enhanced reforming and solar thermochemical energy storage. In this study, we have prepared a series of Li4SiO4 sorbents using a combination of K2CO3 addition and dry ball-milling procedure to improve the relatively slow kinetics under low CO2 partial pressure conditions. The synergistic effects of dry ball-milling and K2CO3 addition on the intrinsic properties of Li4SiO4 sorbents were explored by thermogravimetric analysis and structural characterizations. Thermogravimetric analysis indicate that the highest CO2 uptakes were achieved with dry ball-milling combined with K2CO3 physical addition. The structural characterizations further reveal that this sorbent (P-3K-1.5 M) had the smallest crystallite/particle size, largest surface area, and highest availability of surface alkaline-sites. The kinetics analysis also demonstrates that P-3K-1.5 M exhibited the fastest sorption kinetics during a double process. Additionally, P-3K-1.5 M maintained a high capacity over 10 sorption/desorption cycles. Therefore, this synthesis technique, which is simple, cost-effective, and easily scalable, shows great promise for high-temperature CO2 capture.

正硅酸锂(Li4SiO4)吸附剂对二氧化碳的可逆吸收/解吸为高温烟气中二氧化碳的高温捕集、吸附增强重整和太阳能热化学储能提供了潜力。在本研究中,我们采用添加 K2CO3 和干法球磨相结合的方法制备了一系列 Li4SiO4 吸附剂,以改善其在低二氧化碳分压条件下相对较慢的动力学特性。通过热重分析和结构表征,探讨了干法球磨和添加 K2CO3 对 Li4SiO4 吸附剂内在性质的协同效应。热重分析表明,干法球磨结合 K2CO3 物理添加可实现最高的二氧化碳吸收率。结构表征进一步表明,这种吸附剂(P-3K-1.5 M)的结晶/颗粒尺寸最小,比表面积最大,表面碱性位点的可用性最高。动力学分析还表明,P-3K-1.5 M 在双重过程中表现出最快的吸附动力学。此外,P-3K-1.5 M 还能在 10 次吸附/解吸循环中保持较高的吸附容量。因此,这种合成技术简单、成本效益高且易于扩展,在高温捕获二氧化碳方面大有可为。
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引用次数: 0
Biomimetic mineralization for carbon capture and sequestration 用于碳捕获与封存的仿生矿化技术
Pub Date : 2024-07-27 DOI: 10.1016/j.ccst.2024.100257

Carbon mineralization is an emerging field of research in carbon sequestration. In this process, dissolved inorganic carbon reacts with mineral cations such as Ca2+ and Mg2+ to form stable carbonate minerals, enabling permanent carbon sequestration and storage. However, current mineralization methods predominantly rely on physicochemical approaches to expedite the mineralization of carbon. While effective, these methods require substantial chemical and energy consumption and may cause significant environmental impacts. Biomineralization has recently emerged as a sustainable alternative, leveraging biochemical reactions to catalyze CO2 mineralization. This research focuses on investigating the specific roles of various biomolecules in natural carbon biomineralization and exploring state-of-the-art biomimetic carbon mineralization techniques, including whole-cell microbially induced carbonate precipitation (MICP) and cell-free systems, for carbon sequestration. In addition, we discuss various sources of mineral cations, ranging from natural minerals to industrial waste to seawater, along with their advantages and limitations. Our findings highlight the potential and feasibility of biological carbon mineralization processes to contribute towards sustainable carbon sequestration. However, we also identify challenges and propose future directions to guide further research and the application of these processes.

碳矿化是碳封存的一个新兴研究领域。在这一过程中,溶解的无机碳与 Ca2+ 和 Mg2+ 等矿物阳离子发生反应,形成稳定的碳酸盐矿物,从而实现永久固碳和碳封存。然而,目前的矿化方法主要依靠物理化学方法来加速碳的矿化。这些方法虽然有效,但需要消耗大量的化学物质和能源,并可能对环境造成重大影响。最近出现的生物矿化法是一种可持续的替代方法,它利用生化反应催化二氧化碳矿化。本研究的重点是调查各种生物分子在天然碳生物矿化中的具体作用,并探索最先进的生物模拟碳矿化技术,包括用于碳封存的全细胞微生物诱导碳酸盐沉淀(MICP)和无细胞系统。此外,我们还讨论了从天然矿物、工业废料到海水等各种矿物阳离子来源及其优势和局限性。我们的研究结果凸显了生物碳矿化过程在促进可持续碳固存方面的潜力和可行性。不过,我们也发现了挑战,并提出了未来的方向,以指导进一步的研究和这些过程的应用。
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引用次数: 0
Preparation of high-value carbon nanotubes from real waste plastic towards the negative carbon technology 利用废旧塑料制备高价值碳纳米管,实现负碳技术
Pub Date : 2024-07-26 DOI: 10.1016/j.ccst.2024.100258

The preparation of carbon nanotubes (CNTs) from plastics is of great significance for realizing high value utilization of waste and reducing carbon emission. Here, several kinds of real waste plastics were introduced into catalytic pyrolysis, and the process was also optimized. The results showed that the presence of impurities (e.g., adhesive labels) reduced the initial activation energy of the pyrolysis reaction, and the pyrolysis process was extended and could be divided into two stages. During the catalytic process, impurities play a toxic role on the catalyst at higher temperatures and result in the agglomeration of catalyst particles and a decrease in catalytic activity. Less than 10 wt.% carbon fibers were collected from milk cup waste. However, after experimental optimization, the influence of the impurity component was greatly reduced. The toxic effect of organic impurity volatiles on a catalyst was avoided by employing a segmented catalytic pyrolysis process, which led to an increase in solid carbon content of more than 20 % for express package waste. Simultaneously, more uniform and smoother CNTs can be found in the obtained solid carbon. The process of preparing carbon nanotubes with higher yield and better quality is feasible and has important application prospects in the utilization of waste plastics.

从塑料中制备碳纳米管(CNTs)对于实现废弃物的高值化利用和减少碳排放具有重要意义。本文将几种真实的废塑料引入催化热解,并对工艺进行了优化。结果表明,杂质(如粘胶标签)的存在降低了热解反应的初始活化能,热解过程延长并可分为两个阶段。在催化过程中,杂质在较高温度下对催化剂起毒害作用,导致催化剂颗粒团聚,降低催化活性。从牛奶杯废料中收集的碳纤维重量小于 10%。但经过实验优化后,杂质成分的影响大大降低。通过采用分段催化热解工艺,避免了有机杂质挥发物对催化剂的毒性影响,从而使快递包装垃圾的固体碳含量增加了 20% 以上。同时,在获得的固体碳中可以发现更均匀、更光滑的碳纳米管。制备产量更高、质量更好的碳纳米管的工艺是可行的,在废塑料利用方面具有重要的应用前景。
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引用次数: 0
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Carbon Capture Science & Technology
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