carbon dioxide capture

二氧化碳捕集
  • 文章类型: Journal Article
    温室气体的过度排放,这导致了全球变暖,并警告了世界,引发了全球碳中和运动。碳捕获和封存(CCS)技术作为一种通用的减排技术引起了广泛的研究兴趣。金属有机骨架(MOFs),作为一种新型的高性能吸附剂,由于其超高比表面积和孔隙结构,因此具有从大型点源和环境空气中捕获CO2的巨大潜力。近年来,MOFs在CO2捕集与分离领域取得了很大进展,并发表了一些重要成果,这极大地促进了MOF材料在实际碳捕集应用中的发展。这篇综述总结了过去六年中在各种应用场景中用于碳捕获的MOF材料的最新先进研究。详细描述了增强MOFs的CO2选择性吸附和分离的策略,随着MOF基复合材料的发展。此外,本文还系统地总结了MOF材料在碳捕集实际应用中备受关注的问题。最后,并对未来MOF材料捕集CO2的研究进行了展望。
    The excessive emission of greenhouse gases, which leads to global warming and alarms the world, has triggered a global campaign for carbon neutrality. Carbon capture and sequestration (CCS) technology has aroused wide research interest as a versatile emission mitigation technology. Metal-organic frameworks (MOFs), as a new class of high-performance adsorbents, hold great potential for CO2 capture from large point sources and ambient air due to their ultra-high specific surface area as well as pore structure. In recent years, MOFs have made great progress in the field of CO2 capture and separation, and have published a number of important results, which have greatly promoted the development of MOF materials for practical carbon capture applications. This review summarizes the most recent advanced research on MOF materials for carbon capture in various application scenarios over the past six years. The strategies for enhancing CO2 selective adsorption and separation of MOFs are described in detail, along with the development of MOF-based composites. Moreover, this review also systematically summarizes the highly concerned issues of MOF materials in practical applications of carbon capture. Finally, future research on CO2 capture by MOF materials is prospected.
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  • 文章类型: Journal Article
    在这项研究中,首次用于二氧化碳捕获和利用的创新且具有成本效益的离子聚合物,据报道,使用丰富的非食品生物质木质素。改性的离子聚合物通过缩水甘油基三甲基氯化铵与木质素在碱性条件下的反应来合成以产生季铵离子官能团。随后,基于氢氧化物的纯离子木质素聚合物用于在室温和大气压下从直接空气和浓缩CO2源中捕获CO2。聚合物的结构表征是通过1H,13C,和2D-异核单量子相干(HSQC)NMR,和FT-IR光谱。CO2捕获过程是通过在CO2的存在下形成碳酸氢根离子而建立的。通过使用具有内标(三恶烷)的反向门控质子去耦13CNMR来精确定量捕获的CO2。值得注意的是,离子木质素聚合物的捕获CO2量为来自浓缩CO2源的1.06mmolg-1(47mgg-1)和来自直接空气的0.60mmolg-1(26mgg-1)。离子木质素聚合物中捕获的CO2以可控方式释放并用于环状碳酸酯的合成,展示了捕获碳的生产应用。此外,离子木质素聚合物的完全控制回收通过重复CO2释放↔CO2捕获来实现。
    In this study, an innovative and cost-effective ionic polymer for CO2 capture and utilization for the first time, using abundant and nonfood-based biomass lignin is reported. The modified ionic polymer synthesizes through the reaction of glycidyltrimethylammonium chloride with lignin under alkaline conditions to yield quaternary ammonium ionic functionality. Subsequently, the hydroxide-based pure ionic lignin polymer is employed for CO2 capture from both direct air and concentrated CO2 sources at room temperature and atmospheric pressure. Structural characterization of the polymers is accomplished through 1H, 13C, and 2D-heteronuclear single quantum coherence (HSQC) NMR, and FT-IR spectroscopy. The CO2 capture process is established through the formation of bicarbonate ions alongside the presence of CO2. The captured CO2 is precisely quantified by using inverse-gated proton decoupled 13C NMR with an internal standard (trioxane). Remarkably, the captured-CO2 amounts of ionic lignin polymer are 1.06 mmol g-1 (47 mg g-1) from concentrated-CO2 source and 0.60 mmol g-1 (26 mg g-1) from direct-air. The captured-CO2 in ionic lignin polymer is released in controlled manner and utilized in the synthesis of cyclic carbonate, showcasing the productive application of the captured carbon. Moreover, the fully controlled recovering of ionic lignin polymer achieves via repeated CO2 release ↔ CO2 capture.
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  • 文章类型: Journal Article
    这项工作研究了二氧化碳在浸渍硅胶上的低温吸附。浸渍剂使用聚乙烯亚胺。浸渍剂在硅胶基质中的含量为33.4重量%。%.材料特性,如Brunauer-Emmett-Teller(BET)表面积,孔隙分布,总孔体积,并测定样品的浸渍材料的热稳定性。在吸附-解吸循环的测量过程中,还确定了浸渍剂在材料基质中的损失。由于聚乙烯亚胺含量的减少,吸附剂对CO2的吸附能力也降低。发现在第20次吸附-解吸循环后,浸渍剂在吸附剂中的含量下降了3.15wt。%,and,因此,二氧化碳的吸附能力下降到几乎一半。
    This work studied the low-temperature sorption of carbon dioxide on impregnated silica gel. An impregnating agent was used polyethyleneimine. The content of the impregnating agent in the silica gel matrix was 33.4 wt.%. Material properties such as the Brunauer-Emmett-Teller (BET) surface area, pore distribution, total pore volume, and thermal stability of the impregnated material were determined for the sample. During the measurement of the adsorption-desorption cycles, the loss of the impregnating agent in the material matrix was also determined. Due to the decrease in the content of polyethyleneimine, the sorption capacity of the adsorbent for CO2 also decreased. It was found that after the 20th adsorption-desorption cycle, the content of the impregnating agent in the adsorbent dropped by 3.15 wt.%, and, as a result, the adsorption capacity for CO2 dropped to almost half.
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  • 文章类型: Journal Article
    多孔金属有机骨架(MOFs),也称为多孔配位聚合物,代表一类新的多孔材料,它们的一个显著特征在于它们的可调,可设计,和可功能化的纳米空间。MOFs中的这个纳米空间几乎提供了足够的想象空间,允许不同尺寸的设计合并,形状,以及用于有针对性的气体储存和分离应用的功能。此外,高孔隙率的特点,可调框架结构和孔径,和固定的功能位点使MOF材料能够充分利用其纳米孔空间进行气体储存,为了优化它们的筛分效果,并区分它们与气体分子的相互作用以进行气体分离。在这篇评论文章中,我们强调了最近在开发用于一些最重要的气体储存和分离应用的微孔MOFs方面的一些重大进展。
    Porous metal-organic frameworks (MOFs), also known as porous coordination polymers, represent a new class of porous materials, and one of their striking features lies in their tunable, designable, and functionalizable nanospace. This nanospace within MOFs provides virtually plenty of room for imagination, allowing designed incorporation of different size, shape, and functionalities for targeted gas storage and separation applications. Furthermore, the features of high porosities, tunable framework structures and pore sizes, and immobilized functional sites enable MOF materials to fully make use of their nanopore space for gas storage, to optimize their sieving effects, and to differentiate their interactions with gas molecules for gas separation. In this review article, we highlight some recent significant advances in developing microporous MOFs for some of the most important gas storage and separation applications.
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  • 文章类型: Journal Article
    动力活性炭的使用通常受到粒度和孔隙率不一致的限制,导致吸附效率降低。在这项研究中,我们展示了一种实用且环保的方法,用于通过一系列脱木质素从木质生物质中创建具有高度均匀超微孔的3D石墨烯纳米结构,碳化,和激活过程。此外,我们评估了该结构对CO2,CH4和N2气体的捕获特性以及对二元混合气体的选择性。基于纹理和化学分析,脱木质素的整料具有由纤维素基纤维互连的层状结构。有趣的是,将KOH蒸气活化技术仅应用于脱木质素的样品导致形成由具有高结晶度的互连石墨烯片组成的整体3D网络。尤其是,该法案。1000个样品的比表面积为1480m2/g,孔体积为0.581cm3/g,具有在3.5-11µ范围内超过90%的一致超微孔。基于石墨烯的单片样品,主要由超微孔组成,在110kPa下对CO2的捕获能力显着提高了6.934mol/kg,并且在二元气体混合物(CO2/N2,CO2/CH4和CO2/CH4)中具有良好的选择性。我们的发现表明,这种生物质衍生的3D结构具有在气体分离应用中用作整体吸附剂的潜力。
    The use of powered activated carbon is often limited by inconsistent particle sizes and porosities, leading to reduced adsorption efficiencies. In this study, we demonstrated a practical and environmentally friendly method for creating a 3D graphene nanostructure with highly uniform ultramicropores from wood-based biomass through a series of delignification, carbonization, and activation processes. In addition, we evaluated the capture characteristics of this structure for CO2, CH4, and N2 gases as well as its selectivity for binary-mixture gases. Based on textural and chemical analyses, the delignified monolith had a lamellar structure interconnected by cellulose-based fibers. Interestingly, applying the KOH vapor activation technique solely to the delignified samples led to the formation of a monolithic 3D network composed of interconnected graphene sheets with a high degree of crystallinity. Especially, the Act. 1000 sample exhibited a specific surface area of 1480 m2/g and a considerable pore volume of 0.581 cm3/g, featuring consistently uniform ultramicropores over 90% in the range of 3.5-11 Å. The monolithic graphene-based samples, predominantly composed of ultramicropores, demonstrated a notably heightened capture capacity of 6.934 mol/kg at 110 kPa for CO2, along with favorable selectivity within binary gas mixtures (CO2/N2, CO2/CH4, and CO2/CH4). Our findings suggest that this biomass-derived 3D structure has the potential to serve as a monolithic adsorbent in gas separation applications.
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  • 文章类型: Journal Article
    液相传质是氨水捕集二氧化碳的限速步骤,这导致低的总传质系数和因此差的二氧化碳去除效率。对于这个问题,本研究建立了具有优良传质性能的文丘里反应器,以促进二氧化碳捕获过程中的传质速率,考察了文丘里反应器操作参数对二氧化碳脱除效率和总传质系数的影响。结果表明,随着射流流量从8.31L/min增加到12.73L/min,由于烟气流量的增加,二氧化碳的去除效率下降,随着反应时间的延长,传质系数总体呈由增大到减小的变化趋势。随着氨浓度从0.1wt%增加到0.75wt%,二氧化碳的去除效率和总质量分数系数增加。随着进口二氧化碳浓度从7%增加到19%,二氧化碳的去除效率和整体传质系数下降。文丘里反应器在二氧化碳捕获过程中具有快速的传质速率,在氨浓度为0.75wt%时,最大CO2去除效率为96.4%,CO2体积浓度为15%,射流流速8.36L/min。该研究为二氧化碳捕集文丘里反应器的开发提供了理论价值。
    Mass transfer in liquid phase is the rate-limiting step for carbon dioxide capture by ammonia water, which results in a low total mass transfer coefficient and thus a poor carbon dioxide removal efficiency. For this issue, this study established a venturi reactor with an excellent mass transfer performance to promote mass transfer rate during carbon dioxide capture, and investigated the effect of operating parameters of the venturi reactor on carbon dioxide removal efficiency and overall mass transfer coefficient. The results showed that with an increasing flow rate of the jet from 8.31 to 12.73 L/min, the carbon dioxide removal efficiency decreased due to the increase of flow rate of flue gas, and the changing trend of overall mass transfer coefficient gradually transited from increasing to decreasing with the extension of reaction time. The carbon dioxide removal efficiency and the overall mass fraction coefficient increased upon the increase of ammonia concentration from 0.1 wt% to 0.75 wt%. With the increase of inlet carbon dioxide concentration from 7% to 19%, the carbon dioxide removal efficiency and the overall mass transfer coefficient decreased. Venturi reactor was of a fast mass transfer rate during carbon dioxide capture, and the maximum CO2 removal efficiency was 96.4% at ammonia concentration of 0.75 wt%, CO2 volume concentration of 15%, flow rate of jet of 8.36 L/min. This study provided a theoretical value for the development of venturi reactor for carbon dioxide capture.
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  • 文章类型: Journal Article
    碳酸酐酶(CA)作为一种绿色高效的生物催化剂在CO2捕集领域具有广阔的应用前景。并且已经报道了许多固定CA的成功案例。然而,很少报道用于CO2封存的金属上的CA防污涂层。在这里,二聚CA,来自带有铁蛋白标签的偶氮硫氢(SazCA),它是通过低速离心以高产率制备的,作为游离酶采用并封装在溶胶-凝胶二氧化硅中。将二氧化硅固定的CA分散到商业化的金属防污环氧树脂涂料中,以获得CA涂层的镍泡沫,具有出色的稳定性,在30°C和60°C下孵育28天后,残留活性为90%和67%,分别。CA涂覆的镍泡沫在28天内使用6次循环后保持60%的原始活性。然后,使用CA涂覆的镍泡沫和小球藻构建CA-微藻碳捕获装置。培养7天后,小球藻的生长速率显著增加,小球藻的生物量与对照相比增加29%。由于制备工艺简单,成本效益高,可持续和高效的二氧化碳吸收,这种易于放大的CA涂层镍泡沫在CA辅助微藻的CO2捕获和碳中和方面具有巨大的潜力。
    Carbonic anhydrase (CA) has a promising application as a green and efficient biocatalyst for CO2 capture, and many successful cases of immobilizing CA have been reported. However, CA antifouling coatings on metal for CO2 sequestration have rarely been reported. Herein, dimeric CA from Sulfurihydrogenibium azorense (SazCA) with a ferritin tag, which was prepared by low-speed centrifugation with high yield, was adopted as a free enzyme and encapsulated in the sol-gel silica. The silica-immobilized CAs were dispersed into the commercialized metal-antifouling epoxy resin paint to obtain CA coated nickel foams, which had excellent stability, with 90 % and 67 % residual activity after 28 days of incubation at 30 °C and 60 °C, respectively. The CA coated nickel foams remained 60 % original activity after 6 cycles of use within 28 days. Then, a CA-microalgae carbon capture device was constructed using the CA coated nickel foams and Chlorella. The growth rate of Chlorella was significantly increased and the biomass of Chlorella increased by 29 % compared with control after 7 days of incubation. Due to the simple and cost-effective preparation process, sustainable and efficient CO2 absorption, this easy-to-scale up CA coated nickel foam has great potential in CA assisted microalgae-based CO2 capture and carbon neutrality.
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  • 文章类型: Journal Article
    活性炭是一种有吸引力的吸附剂,用于捕获各种环境污染物,包括CO2。在这里,据报道,由Balanitesagyptiaca(沙漠日期)种子壳制成的活性炭的最佳合成和令人印象深刻的性能,这是中东和非洲丰富的农业废物。合成途径涉及用KOH预处理生物质并在合适的温度分布下加热。最佳的KOH与生物质的比例和多级碳化产生的活性炭的表面积超过3000m2/g,平均孔径近4.1nm。在0°C时,这种活性炭的CO2吸收量为11.3mmol·g-1,超过了以前报道的活性炭的吸收能力。还发现与其它气体相比,对CO2的选择性显著更高。因此,本方法证明了农业废物向活性炭的有效转化,以捕获CO2和其它环境污染物。
    Activated carbon is an attractive adsorbent for capturing various environmental pollutants, including CO2. Herein, an optimal synthesis and impressive performance of activated carbon made from Balanites aegyptiaca (Desert date) seed shells is reported, which is an abundant agricultural waste in the Middle East and Africa. The synthesis route involved pretreating the biomass with KOH and heating it under a suitable temperature profile. An optimal KOH-to-biomass ratio and multi-stage carbonization yielded activated carbon with a surface area above 3000 m2/g and an average pore size of nearly 4.1 nm. At 0 °C, this activated carbon exhibited CO2 uptake of 11.3 mmol g-1 that surpassed the uptake capacity of previously reported activated carbons. The selectivity towards CO2 was also found to be significantly higher compared to other gases. Thus, the present approach demonstrates an efficient conversion of agricultural waste to activated carbon for capturing CO2 and other environmental contaminants.
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  • 文章类型: Journal Article
    共价有机骨架是一类新型的结晶多孔聚合物,其使得延伸的多边形骨架的分子设计能够获得良好限定的多孔结构。然而,构建允许远程控制毛孔的框架仍然是一个挑战。在这里,我们报告了一种共价合并的策略,非共价,和光化学来设计具有可逆和远程可控孔的光响应框架。我们开发了一种拓扑引导的多组分缩聚系统,该系统以预先设计的密度将突出的四氟偶氮苯单元作为光响应位点整合在孔壁上,因此,可以构建具有相同主链的一系列结晶多孔骨架,以形成从中孔到微孔的宽范围的孔。与传统的偶氮苯体系不同,四氟偶氮苯骨架对可见光高度敏感以进行高速率异构化。光异构化对孔径产生深远的影响,形状,number,和环境,以及分子的摄取和释放,渲染系统能够转换和切换孔可逆和远程可见光。我们的研究结果为一类具有孔结构和功能的新型智能多孔材料开辟了道路,这些孔结构和功能可以用可见光转换和管理。
    Covalent organic frameworks are a novel class of crystalline porous polymers that enable molecular design of extended polygonal skeletons to attain well-defined porous structures. However, construction of a framework that allows remote control of pores remains a challenge. Here we report a strategy that merges covalent, noncovalent, and photo chemistries to design photoresponsive frameworks with reversibly and remotely controllable pores. We developed a topology-guided multicomponent polycondensation system that integrates protruded tetrafluoroazobenzene units as photoresponsive sites on pore walls at predesigned densities, so that a series of crystalline porous frameworks with the same backbone can be constructed to develop a broad spectrum of pores ranging from mesopores to micropores. Distinct from conventional azobenzene-based systems, the tetrafluoroazobenzene frameworks are highly sensitive to visible lights to undergo high-rate isomerization. The photoisomerization exerts profound effects on pore size, shape, number, and environment, as well as molecular uptake and release, rendering the system able to convert and switch pores reversibly and remotely with visible lights. Our results open a way to a novel class of smart porous materials with pore structures and functions that are convertible and manageable with visible lights.
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  • 文章类型: Journal Article
    非水吸收剂(NAAs)由于其巨大的节能潜力而吸引了越来越多的人们对CO2捕集的关注。可以提供高CO2吸收负载的伯二胺是用于配制NAA的有希望的候选物,但在再生能力方面具有缺点。在这项研究中,提出了一种有希望的策略,即使用叔胺(TA)作为质子转移介质来增强氨基乙基乙醇胺的可再生性(AEEA,二胺)/二甲基亚砜(DMSO)(A/D)NAA。令人惊讶的是,一些采用的TA,如N,N-二乙基氨基乙醇(DEEA),N,N,N\',N\'\',N\'\'-五甲基二亚乙基三胺(PMDETA),3-二甲基氨基-1-丙醇(3DMA1P),N,N-二甲基乙醇胺(DMEA)不仅提高了A/DNAA的再生能力,而且还提高了CO2吸收性能。具体来说,CO2吸收负荷和循环负荷分别增加了约12.7%和15.5%-22.7%,分别。通过核磁共振技术和量子化学计算,全面探索了TA增强的CO2捕集机理。在CO2吸收过程中,TA充当AEEA-两性离子的最终质子受体,并使更多的AEEA形成氨基甲酸酯物种(AEEACOO-)来存储CO2,从而增强CO2吸收。对于CO2解吸,TA首先直接向AEEACOO-作为质子供体提供质子;此外,它充当质子载体,并促进了从质子化AEEA到AEEACOO-的低能逐步质子转移。因此,TA的存在使AEEACOO-更容易获得质子分解,导致CO2解吸增强。一句话,在A/DNAA中引入TA作为质子转移介质,提高了CO2吸收性能和再生能力,这是“一石二鸟”的有效方法。
    Non-aqueous absorbents (NAAs) have attracted increasing attention for CO2 capture because of their great energy-saving potential. Primary diamines which can provide high CO2 absorption loading are promising candidates for formulating NAAs but suffer disadvantages in regenerability. In this study, a promising strategy that using tertiary amines (TAs) as proton-transfer mediators was proposed to enhance the regenerability of an aminoethylethanolamine (AEEA, diamine)/dimethyl sulfoxide (DMSO) (A/D) NAA. Surprisingly, some employed TAs such as N,N-diethylaminoethanol (DEEA), N,N,N\',N\'\',N\'\'-pentamethyldiethylenetriamine (PMDETA), 3-dimethylamino-1-propanol (3DMA1P), and N,N-dimethylethanolamine (DMEA) enhanced not only the regenerability of the A/D NAA but also the CO2 absorption performance. Specifically, the CO2 absorption loading and cyclic loading were increased by about 12.7% and 15.5%-22.7%, respectively. The TA-enhanced CO2 capture mechanism was comprehensively explored via nuclear magnetic resonance technique and quantum chemical calculations. During CO2 absorption, the TA acted as an ultimate proton acceptor for AEEA-zwitterion and enabled more AEEA to form carbamate species (AEEACOO-) to store CO2, thus enhancing CO2 absorption. For CO2 desorption, the TA first provided protons directly to AEEACOO- as a proton donor; moreover, it functioned as a proton carrier and facilitated the low-energy step-wise proton transfer from protonated AEEA to AEEACOO-. Consequently, the presence of TA made it easier for AEEACOO- to obtain protons to decompose, resulting in enhanced CO2 desorption. In a word, introducing the TA as a proton-transfer mediator into the A/D NAA enhanced both the CO2 absorption performance and the regenerability, which was an efficient way to \"kill two birds with one stone\".
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