共查询到17条相似文献，搜索用时 78 毫秒
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综述了近年来离子液体介质中CO2电活化合成有机碳酸酯的研究进展, 着重概述了电催化合成碳酸二甲酯(DMC)和环状碳酸酯的研究现状, 并简述了CO2间接电活化和直接电活化技术, 以及反应介质、电极材料等因素对反应产物的影响, 对电催化还原CO2的关键技术和今后研究重点进行了探讨。离子液体具有不易挥发、可循环使用、导电性好、对CO2有较高溶解度等优点, 在CO2固定和有机资源化研究中日益受到重视。电化学作为一种环境友好的绿色合成新技术, 在CO2有机资源化方面有很好的应用前景, 对缓解日益严峻的温室效应、实现CO2的资源化利用具有十分重要的现实意义。 相似文献
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二氧化碳（CO2）捕集、利用和储存（CCUS）在全球能源结构转型中是一种极具潜力的策略,能够实现能源供给、基础原料产出以及限制气候变化。多孔有机聚合物（POPs）具有高CO2吸附容量和吸附选择性、突出的结构特性以及优异的化学可调控性,其作为极具潜力的材料广泛应用于催化CO2参与的有机反应中。其中,CO2与环氧化物环加成生成环状碳酸酯的反应具有100%的原子经济性,且其产物也极具工业价值。本文基于CO2环加成反应催化机制,从催化剂的合成方法、结构性质与组成特性角度出发,综述了POPs在CO2/环氧化物环加成反应的研究进展,包括金属配合物类、氢键供体类、离子液体类、金属配合物/离子液体和氢键供体/离子液体等有机多孔聚合物体系。通过阐述POPs在催化CO2制备高附加值环状碳酸酯反应中的研究现状和发展趋势,为POPs的开发与应用以及CO2综合利用的工业化探索提供具有建设性的指导意见。 相似文献
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CO2作为一种温室气体,是一种宝贵的C1资源,为实现“碳达峰、碳中和”战略目标,大力发展二氧化碳利用与封存技术是当务之急。离子液体是由有机阳离子和有机或无机阴离子组成的绿色溶剂,而低共熔溶剂是由氢键受体和氢键供体通过氢键形成的一种新型的溶剂。离子液体基低共熔溶剂不仅拥有离子液体相似的性质,如低饱和蒸气压、宽液温范围、高热化学稳定性、结构性能可调控等,还具备了低共熔溶剂的氢键特性。本文综述了离子液体基低共熔溶剂在CO2热催化、电催化、生物催化领域的应用,并分析了各种催化方式中的CO2转化机理和影响因素,展望了低共熔溶剂应用于转化CO2的前景,对目前该领域的发展所面临的主要问题和进一步的研究工作提出了建议。 相似文献
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离子液体(ILs)和低共熔溶剂(DESs)作为一类新型的绿色溶剂,由于其独特的物理化学性质,在混合物分离方面已经受到了研究者的广泛关注,因此逐渐成为绿色化学领域的研究重点。针对特定的分离过程,选择合适的溶剂是非常重要的,然而,由于ILs和DESs种类较多,结构复杂,通过实验的方法逐一进行筛选费时费力、成本高,且几乎不可能找到最优选择,因此应用理论计算模型对ILs和DESs进行筛选是非常有必要的。真实溶剂类导体屏蔽模型(COSMO-RS模型)是一种由量子化学计算与统计热力学方法相结合的预测模型,它可以在不需要实验数据的情况下预测液体混合物的热力学性质,已经被研究者广泛用作各种分离问题的快速筛选工具。整理了应用COSMO-RS模型筛选ILs/DESs用于各种油中酚类、含氮化合物、含硫化合物、萜类化合物、天然维生素E的萃取分离,以及CO2捕获和共沸混合物等的分离过程,表明COSMO-RS模型用于特定混合物萃取溶剂的筛选是快速有效的,可为难分离混合物分离过程中ILs/DESs的预筛选提供有价值的参考。 相似文献
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为了实现煤基液体各组分利用价值最大化,本文综述了离子液体和低共熔溶剂对组分组成复杂的煤基液体进行高效萃取分离的研究进展。首先介绍了离子液体和低共熔溶剂的性质及分类;其次根据分离目标的不同,将离子液体和低共熔溶剂对煤基液体典型组分的萃取分离分为四个方面进行阐述:煤基液体提酚、燃料油萃取脱硫、燃料油萃取脱氮、芳烃和脂肪烃的分离。分析表明,离子液体和低共熔溶剂对实际煤基液体的提酚效果较好,能分离出绝大多数的酚类化合物;燃料油萃取脱硫时,离子液体和低共熔溶剂对实际煤基液体的单次脱硫率均不高,需3～5次重复萃取后才能获得理想效果;燃料油中的碱性及非碱性含氮化合物很难被同一种离子液体或低共熔溶剂一次性分离出,导致实际油品的脱氮率较低;大多数离子液体和低共熔溶剂进行芳烃和脂肪烃的分离时不能获得理想的分配系数和选择性,尚无法用于实际芳烃和脂肪烃的分离。氢键、π-π、CH-π、范德华力等分子间相互作用的差异是实现离子液体或低共熔溶剂进行煤基液体典型组分分离的主要原因。依据分离对象,设计合适的离子液体和低共熔溶剂,提高实际煤基液体分离时的萃取率和选择性;分析并解决离子液体和低共熔溶剂用于实际煤基液体各组分... 相似文献
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考察了碱性离子液体催化碳酸二甲酯和乙醇酯交换反应合成碳酸甲乙酯的过程, 筛选出催化性能较好的离子液体1-丁基-3-甲基咪唑溴盐（［Bmim］Br）作为催化剂, 并对酯交换反应条件进行优化。结果表明,［Bmim］Br对反应表现出优异的催化性能,在常压、反应温度90 ℃、反应时间12 h、n(碳酸二甲酯)∶n(乙醇)=1∶1和［Bmim］Br用量为碳酸二甲酯质量的2%条件下,碳酸二甲酯转化率为71.1%,碳酸甲乙酯选择性为81.8%。经回收和循环利用 3次,催化剂仍保持较好的催化活性。 相似文献
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氨气（NH3）作为一种有害气体,其传统吸收技术存在诸多缺陷,亟需开发性能优越的NH3吸收剂,以开发新型NH3分离技术。离子液体和低共熔溶剂作为气体分离过程的潜在吸收剂,因低挥发性、良好的热稳定性以及灵活的可调控性等特点受到越来越多的关注。但离子液体和低共熔溶剂数量众多,筛选困难。采用热力学分析方法分析离子液体和低共熔溶剂用于NH3分离过程,基于Gibbs自由能变,拟合出分离过程的最佳操作条件,将总能耗和离子液体用量作为筛选标准,筛选出性能良好的[Omim][BF4]。将[Omim][BF4]与传统NH3吸收剂水对比,发现[Omim][BF4]具有更低的能耗。最后,拟合出筛选标准与离子液体/低共熔溶剂的临界性质间的规律,为开发新的NH3吸收剂和新的分离技术提供依据。 相似文献
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合成了咪唑离子液体功能化salen Mn配合物（IL-salen Mn）,并作为唯一催化剂成功应用于苯乙烯与二氧化碳一锅合成碳酸苯乙烯酯反应中。首先,以尿素过氧化氢（UHP）为氧化剂、吡啶氮氧化物（PyNO）为助剂,催化苯乙烯高效制备环氧苯乙烷,继而催化环氧苯乙烷与二氧化碳发生环加成反应合成碳酸苯乙烯酯。分别考察了催化剂的种类和用量、助剂用量、氧化剂种类和用量、反应时间以及反应温度等因素对上述反应的影响。当催化剂用量为8 mol%（以反应物总的物质的量记）,n(苯乙烯)∶n(UHP)∶n(PyNO)=1.0∶3.0∶0.2,环氧化反应温度和时间分别为30 ℃和5 h,环加成反应温度和时间分别为80 ℃和12 h,二氧化碳压力为1 MPa时,苯乙烯的转化率为90%,碳酸苯乙烯酯收率达到32%。结合前期研究与反应时间动力学结果,推测了该串联反应可能的机理。 相似文献
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L. F. Zubeir P. J. L. Lipman J. van der Schaaf N. Awwad C. J. Peters M. C. Kroon 《American Institute of Chemical Engineers》2017,63(7):2981-2986
A modified version of a standard device for measuring gas adsorption and desorption isotherms and surface area of adsorbents and catalysts (ASAP (Accelerated Surface Area and Porosimetry System) 2020, Micromeritics USA) is used for the first time to measure gas solubilities (i.e., CO2) in low vapor pressure liquids (i.e., the IUPAC standard ionic liquid 1‐hexyl‐3‐methylimidazolium bis(trifluoromethylsulfonyl)imide ([C6mim][Tf2N])) in the Henry's law region. The solubility data are in very good agreement with the reported data in literature. Furthermore, the Henry's law constants are calculated from the solubility data and compared to the experimental data found in literature. The results from this study demonstrate that Micromeritics ASAP 2020 is a suitable apparatus for gas absorption by solvents with reduced vapor pressures. © 2017 American Institute of Chemical Engineers AIChE J, 63: 2981–2986, 2017 相似文献
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胆碱类低共融溶剂是一种新型的离子液体。它不仅具有传统离子液体的优点,还具有价格低廉、低毒、生物可降解等优势。对胆碱类低共融溶剂在CO2捕集与分离中所涉及的物理性质,如气体的溶解度、CO2的吸收-解吸、密度、稳定性、黏度和表面张力等进行考察,并分析了胆碱类低共融溶剂的结构对各物性的影响。通过与传统离子液体的对比,胆碱类低共融溶剂在CO2捕集与分离中的应用具有一定的优势,如CO2溶解度高,黏度低。然而,胆碱类低共融溶剂在气体的选择性分离、表面张力等的研究还不足,且热稳定性方面还存在瓶颈,因此,其在CO2捕集和分离中的应用还有待进一步探讨。 相似文献
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Marina Cvjetko Bubalo Senka Vidović Ivana Radojčić Redovniković Stela Jokić 《Journal of chemical technology and biotechnology (Oxford, Oxfordshire : 1986)》2015,90(9):1631-1639
In many industrial processes, large quantities of volatile and flammable organic solvents are used in various reaction systems and separation steps defining a major part of the environmental and economic performance of a process. Accordingly, a growing area of research in the development of green technologies is devoted to designing new, environment‐friendly and tunable solvents the use of which would meet both technological and economic demands. Among proposed solvents, room temperature ionic liquids, supercritical and subcritical fluids and solvents from natural and renewable sources stand out as the most promising approaches for current solvent innovation. A brief overview of up‐to‐date knowledge regarding these solvents is presented herein, with special emphasis on their properties, applications and further perspectives as truly green industrial solvents. © 2015 Society of Chemical Industry 相似文献
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George M. Neville;Ana-Maria Dobre;Gavin J. Smith;Samantha Micciulla;Nick J. Brooks;Thomas Arnold;Tom Welton;Karen J. Edler; 《Advanced Synthesis u0026amp; Catalysis》2024,34(4):2306644
Mixtures between choline and geranic acid (CAGE) have previously been shown to insert into lipid bilayers. This may be useful for the transdermal delivery of larger pharmaceuticals, however, little is known about the mechanism of activity. By comparing the interactions between CAGE and lipid bilayers with those of a less-active, yet closely-related analogue, choline octanoic acid (CAOT), a chemical basis can be investigated. Overall, six systems are studied here by neutron reflectivity, where d54-1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC) solid-supported phospholipid bilayers are first formed on SiO2 substrates before exposure to the deep eutectic solvent (DES). Components of the DES could be identified within the bilayer by exploiting contrast variation and selective deuteration. CAGE is shown to be a mild disruptive agent, free to insert and diffuse across the bilayer, preserving much of the bilayer integrity. Experiments identify co-mingling of geranate ions inhibits the efficient packing of lipid tails, increasing hydration across the bilayer. Conversely, CAOT is found to both exchange and remove lipid molecules to achieve incorporation, inducing swelling and the formation of solvent patches. It appears these behaviors derive from the structures of the anions and thus amphiphilicity of the DES, laying the foundations for the rational design and optimization of these candidates toward transdermal delivery. 相似文献
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George M. Neville;Ana-Maria Dobre;Gavin J. Smith;Samantha Micciulla;Nick J. Brooks;Thomas Arnold;Tom Welton;Karen J. Edler; 《Advanced Synthesis u0026amp; Catalysis》2024,34(2):2306644
Mixtures between choline and geranic acid (CAGE) have previously been shown to insert into lipid bilayers. This may be useful for the transdermal delivery of larger pharmaceuticals, however, little is known about the mechanism of activity. By comparing the interactions between CAGE and lipid bilayers with those of a less-active, yet closely-related analogue, choline octanoic acid (CAOT), a chemical basis can be investigated. Overall, six systems are studied here by neutron reflectivity, where d54-1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC) solid-supported phospholipid bilayers are first formed on SiO2 substrates before exposure to the deep eutectic solvent (DES). Components of the DES could be identified within the bilayer by exploiting contrast variation and selective deuteration. CAGE is shown to be a mild disruptive agent, free to insert and diffuse across the bilayer, preserving much of the bilayer integrity. Experiments identify co-mingling of geranate ions inhibits the efficient packing of lipid tails, increasing hydration across the bilayer. Conversely, CAOT is found to both exchange and remove lipid molecules to achieve incorporation, inducing swelling and the formation of solvent patches. It appears these behaviors derive from the structures of the anions and thus amphiphilicity of the DES, laying the foundations for the rational design and optimization of these candidates toward transdermal delivery. 相似文献
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Yongkang Cao Xiangping Zhang Shaojuan Zeng Yanrong Liu Haifeng Dong Chun Deng 《American Institute of Chemical Engineers》2020,66(8):e16253
The emerging of ionic liquids (ILs) provides an efficient and sustainable way to separate and recover NH3 due to their unique properties. However, the solid or highly viscous ILs are not suitable for traditional scrubbing. Therefore, an effective strategy was proposed by combining the protic ILs (PILs) with acidic H and low viscous ethylene glycol (EG) to form IL-based deep eutectic solvents (DESs) for NH3 absorption. The results indicated that these PIL-based DESs not only have fast absorption rate, but also exhibit exceptional NH3 capacity and excellent recyclability. The highest mass capacity of 211 mg NH3/g DES was achieved by [Im][NO3]/EG with molar ratio of 1:3, and was higher than all the reported ILs and IL-based DESs, which was originated from multiple hydrogen bonding between acidic H and hydroxyl groups of the DESs and NH3. This work will provide useful idea for designing IL-based solvents for NH3 separation applications. 相似文献
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Ali Aminian 《American Institute of Chemical Engineers》2022,68(9):e17774
This study aims to use perturbed-chain statistical associating fluid theory (PC-SAFT) to describe the phase behavior of systems containing deep eutectic solvents (DESs) and ionic liquids (ILs). The DESs are based on tetrabutylammonium chloride and tetrabutylammonium bromide as hydrogen bond acceptors, and levulinic acid and diethylene glycol as hydrogen bond donors in the mole ratio of 1:2 and 1:4, respectively. Predictions of phase equilibria by PC-SAFT were compared with the results of COnductor like Screening MOdel for Real Solvents (COSMO-RS) and non-random two-liquid (NRTL). In this work, low viscosity ether- and pyridinium-based ILs [EnPy][NTf2] and [CmPy][NTf2] were used for vapor–liquid equilibrium systems, while 1-(2-methoxyethyl)-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)-amide and 1-propyl-3-methylimidazolium bis{trifluoromethylsulfonyl}imide with n-heptane + thiophene and n-hexane + ethylbenzene were used in the liquid–liquid extraction, respectively. In the last part, the phase behavior of the mixtures of perfluoroalkylalkanes with their linear alkane counterparts was studied and compared with the SAFT-Mie pair potential. 相似文献