- Room-temperature molten salt polymers as a matrix for fast ion conduction
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Vinyl polymers having either imidazolium group or sulfonamide group in the side chain were prepared as components to form a molten salt. After mixing, these polymers formed a molten-salt-like flexible domain in the polymer, and excellent ionic conductivity (7.52 X 10-6 Scm-1 and 1.88 X 10-4 Scm-1 at 30°C, respectively) was observed in spite of their rubber-or powder-like properties.
- Ohno, Hiroyuki,Ito, Kaori
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- Lower Activation Energy for Catalytic Reactions through Host–Guest Cooperation within Metal–Organic Frameworks
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Industrial synthesis is driven by a delicate balance of the value of the product against the cost of production. Catalysts are often employed to ensure product turnover is economically favorable by ensuring energy use is minimized. One method, which is gaining attention, involves cooperative catalytic systems. By inserting a flexible polymer into a metal–organic framework (MOF) host, the advantages of both components work synergistically to create a composite that efficiently fixes carbon dioxide to transform various epoxides into cyclic carbonates. The resulting material retains high yields under mild conditions with full reusability. By quantitatively studying the kinetic rates, the activation energy was calculated, for a physical mixture of the catalyst components to be about 50 % higher than that of the composite. Through the unification of two catalytically active components, a new opportunity opens up for the development of synergistic systems in multiple applications.
- Aguila, Briana,Sun, Qi,Wang, Xiaoliang,O'Rourke, Erica,Al-Enizi, Abdullah M.,Nafady, Ayman,Ma, Shengqian
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- Efficient heterogeneous functionalized polymer ionic liquid catalyst for the synthesis of ethylene carbonate via the coupling of carbon dioxide with ethylene oxide
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A series of functionalized polymer ionic liquids (PILs) were synthesized and immobilized onto a 4 A molecular sieve. The catalytic activity of the resulting heterogeneous catalyst toward the synthesis of ethylene carbonate (EC) via the cycloaddition reaction of ethylene oxide (EO) and CO2 was studied. The effects of the reaction conditions such as reaction temperature, pressure, time, and the amount of catalyst used, were systematically investigated. A high yield of EC and excellent selectivity could be obtained under optimized conditions. The catalyst is thermally stable and shows good reusability. Based on the experimental results, a plausible reaction mechanism has been proposed for the catalytic reaction. This journal is the Partner Organisations 2014.
- Zhang, Bo,Zhang, Lei,Wu, Qinghai,Wang, Quanxi,Song, Baoan,Wu, Wenjun,Lu, Bin,Ren, Tianrui
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- Tailoring the Pore Size and Chemistry of Ionic Ultramicroporous Polymers for Trace Sulfur Dioxide Capture with High Capacity and Selectivity
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Here we demonstrate the deep removal of SO2 with high uptake capacity (1.55 mmol g?1) and record SO2/CO2 selectivity (>5000) at ultra-low pressure of 0.002 bar, using ionic ultramicroporous polymers (IUPs) with high density of basic anions. The successful construction of uniform ultramicropores via polymerizing ionic monomers into IUPs enables the fully exploitation of the selective anionic sites. Notably, the aperture size and surface chemistry of IUPs can be finely tuned by adjusting the branched structure of ionic monomers, which play critical roles in excluding CH4 and N2, as well as reducing the coadsorption of CO2. The swelling property of IUPs with adsorption of SO2 contributed to the high SO2 uptake capacity and high separation selectivity. Systematic investigations including static gas adsorption, dynamic breakthrough experiments, stability tests and modeling studies confirmed the efficient performance of IUPs for trace SO2 capture.
- Suo, Xian,Yu, Ying,Qian, Siheng,Zhou, Lin,Cui, Xili,Xing, Huabin
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- Rhodium nanoparticles stabilized by ionic copolymers in ionic liquids: Long lifetime nanocluster catalysts for benzene hydrogenation
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Novel ionic liquid-soluble ionic copolymers containing imidazolium ionic liquidlike units have been synthesized. Rhodium nanoparticles stabilized by the ionic copolymer in ionic liquids have been successfully obtained. The nanoparticles showed unprecedented lifetime and activity in arene hydrogenation under forcing conditions (a temperature of 75 °C and a hydrogen pressure of 40 bar) with a total turnover (TTO) of 20000 (in five total recycles of 4000 TTOs each) and a turnover frequency of 250 h-1, demonstrating that the combination of ionic liquids with ionic liquidlike stabilizers is a pathway towards highly stable and active nanoparticle catalysts. Copyright
- Mu, Xin-Dong,Meng, Jian-Qiang,Li, Zi-Chen,Kou, Yuan
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- Poly(ionic liquid) binders as Li+ conducting mediators for enhanced electrochemical performance
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A series of poly(ionic liquid)s (PILs) were used as binders for lithium-ion battery (LIB) with a LiFePO4 cathode to explore their role and benefits in a model electrochemical energy storage system. The PILs are imidazolium-based and bear differ
- Lee, Jung-Soo,Sakaushi, Ken,Antonietti, Markus,Yuan, Jiayin
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- Poly(ionic liquid) and macrocyclic polyoxometalate ionic self-assemblies: New water-insoluble and visible light photosensitive catalysts
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Several poly(ionic liquid)s (PILs) were synthesized and assembled with a multielectronic-process sustaining polyoxometalate (POM) into new green and water-insoluble nanomaterials (POM@PILs). They are visible light photosensitive, unlike their two componen
- Biboum, Rosa Ngo,Doungmene, Floriant,Keita, Bineta,De Oliveira, Pedro,Nadjo, Louis,Lepoittevin, Benedicte,Roger, Philippe,Brisset, Francois,Mialane, Pierre,Dolbecq, Anne,Mbomekalle, Israel M.,Pichon, Celine,Yin, Panchao,Liu, Tianbo,Contant, Roland
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- Synthesis of anion-functionalized mesoporous poly(ionic liquid)s: Via a microphase separation-hypercrosslinking strategy: Highly efficient adsorbents for bioactive molecules
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The synthesis of porous materials with a well-defined pore structure and functionality is centrally important for the development of advanced adsorbents and sensors. In this study, we explore a direct and facile methodology combining microphase separation and hypercrosslinking, and prepare anion-functionalized mesoporous poly(ionic liquid)s (MPILs) with well-developed mesopores. This methodology involved a copolymerization of IL monomers and crosslinkers to create mesopores via microphase separation. Additionally, the MPILs were texturally engineered by hypercrosslinking to stabilize/rebuild labile collapsed mesoporous networks and generate microporosity. Thus, a new family of anion-functionalized MPILs containing amphiphilic long-chain carboxylate ionic liquids (LCC-ILs) were synthesized. These anion-functionalized MPILs exhibited extraordinarily high adsorption capacity (211.45 mg g-1 for tocopherols) and excellent selectivity (Sδ/α, 8.65; Sβγ/α, 4.20) for bioactive tocopherol homologues and organic phenolic compounds with high structural similarity, significantly better than those of commercial adsorbents or common MPILs. Additionally, anion-functionalized MPILs demonstrated enhanced carbon dioxide (CO2) capture performances (28.18 mg g-1 at 0 °C and 1 bar). This study demonstrates the great potential of anion-functionalized MPILs as advanced adsorbents, and facilitates a textural engineering approach to the development of novel porous ionic materials for other applications.
- Suo, Xian,Xia, Ling,Yang, Qiwei,Zhang, Zhiguo,Bao, Zongbi,Ren, Qilong,Yang, Yiwen,Xing, Huabin
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- Influence of tethered ions on electric polarization and electrorheological property of polymerized ionic liquids
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Polymerized ionic liquids (PILs) show potential to be used as new water-free polyelectrolyte-based electrorheological (ER) material. To direct ER material design at the molecular level, unveiling structure-property relationships is essential. While a few studies compare the mobile ions in PILs there is still a limited understanding of how the structure of tethered counterions on backbone influences ER property. In this study, three PILs with same mobile anions but different tethered countercations (e.g., poly(dimethyldiallylammonium) P[DADMA]+, poly(benzylethyl) trimethylammonium P[VBTMA]+, and poly(1-ethyl-4-vinylimidazolium hexafluorophosphate) P[C2VIm]+) are prepared and the influence of tethered countercations on the ER property of PILs is investigated. It shows that among these PILs, P[DADMA]+ PILs have the strongest ER property and P[C2VIm]+ PILs have the weakest one. By combining dielectric spectra analysis with DFT calculation and activation energy measurement, it can clarify that the influence of tethered counterions on ER property is mainly associated with ion-pair interaction energy that is affecting ionic conductivity and interfacial polarization induced by ion motion. P[DADMA]+ has the smallest ion-pair interaction energy with mobile ions, which can result in the highest ionic conductivity and the fastest interfacial polarization rate for its strongest ER property.
- He, Fang,Wang, Bo,Yin, Jianbo,Zhao, Jia,Zhao, Xiaopeng
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- Incorporation of Imidazolium-Based Poly(ionic liquid)s into a Metal-Organic Framework for CO2 Capture and Conversion
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The rational integration of multiple functional components into a composite material could result in enhanced activity tailored for specific applications. Herein, imidazolium-based poly(ionic liquid)s (denoted as polyILs) have been confined into the metal-organic framework (MOF) material MIL-101 via in situ polymerization of encapsulated monomers. The resultant composite polyILs@MIL-101 exhibits good CO2 capture capability that is beneficial for the catalysis of the cycloaddition of CO2 with epoxides to form cyclic carbonates at subatmospheric pressure in the absence of any cocatalyst. The significantly enhanced activity of polyILs@MIL-101, compared to either MIL-101 or polyILs, is attributed to the synergistic effect among the good CO2 enrichment capacity, the Lewis acid sites in the MOF, as well as the Lewis base sites in the polyILs.
- Ding, Meili,Jiang, Hai-Long
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- Synthesis of polymeric nanoparticles containing reduced graphene oxide nanosheets stabilized by poly(ionic liquid) using miniemulsion polymerization
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Polymeric nanoparticles containing reduced graphene oxide (rGO) nanosheets have been prepared by aqueous miniemulsion radical polymerization of methyl methacrylate (MMA) utilizing poly(ionic liquid) (PIL) as stabilizer to effectively disperse the rGO nanosheets in the monomer phase. The PIL that gave the best results in terms of rGO dispersibility was a block copolymer of the ionic liquid monomer 1-(2-methacryloyloxyethyl)-3-butylimidazolium bis(trifluoromethanesulfonyl)amide ([Mbim][TFSA]) and MMA, the concept being that the MMA units impart solubility in the MMA monomer droplets whereas the IL units act as adsorption sites for rGO. The rGO dispersibility in vinyl monomer was demonstrated to be superior using the above PIL block copolymer compared to the corresponding statistical copolymer or PIL homopolymer. Overall, the approach developed demonstrates how PILs can be employed to conveniently switch (turn ON/OFF) the dispersibility of PIL/rGO via anion exchange reactions, which can be an efficient strategy for synthesis of polymer/rGO nanocomposite materials.
- Tokuda, Masayoshi,Yamane, Mitsuyoshi,Thickett, Stuart C.,Minami, Hideto,Zetterlund, Per B.
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- Flexibility Matters: Cooperative Active Sites in Covalent Organic Framework and Threaded Ionic Polymer
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The combination of two or more reactive centers working in concert on a substrate to facilitate the reaction is now considered state of the art in catalysis, yet there still remains a tremendous challenge. Few heterogeneous systems of this sort have been exploited, as the active sites spatially separated within the rigid framework are usually difficult to cooperate. It is now shown that this roadblock can be surpassed. The underlying principle of the strategy presented here is the integration of catalytic components with excellent flexibility and porous heterogeneous catalysts, as demonstrated by the placement of linear ionic polymers in close proximity to surface Lewis acid active sites anchored on the walls of a covalent organic framework (COF). Using the cycloaddition of the epoxides and CO2 as a model reaction, dramatic activity improvements have been achieved for the composite catalysts in relation to the individual catalytic component. Furthermore, they also clearly outperform the benchmark catalytic systems formed by the combination of the molecular organocatalysts and heterogeneous Lewis acid catalysts, while affording additional recyclability. The extraordinary flexibility and enriched concentration of the catalytically active moieties on linear polymers facilitate the concerted catalysis, thus leading to superior catalytic performance. This work therefore uncovers an entirely new strategy for designing bifunctional catalysts with double-activation behavior and opens a new avenue in the design of multicapable systems that mimic biocatalysis.
- Sun, Qi,Aguila, Briana,Perman, Jason,Nguyen, Nicholas,Ma, Shengqian
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- Efficient fixation of CO2 into cyclic carbonates catalyzed by hydroxyl-functionalized poly(ionic liquids)
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A series of hydroxyl-functionalized poly(ionic liquids) (PILs) were synthesized and employed as catalysts for the synthesis of cyclic carbonates from CO2 and epoxides without the use of any co-catalyst or organic solvent. It was demonstrated th
- Shi, Tian-Yuan,Wang, Jin-Quan,Sun, Jian,Wang, Ming-Hui,Cheng, Wei-Guo,Zhang, Suo-Jiang
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- Poly(ionic liquid)-polyoxometalate/graphene oxide composites as catalysts for deep desulfurization
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A series of polymer ionic liquid (PIL)-based polyoxometalate (POM) salts were designed and synthesized by an ion exchange method. Then, supported catalysts were prepared by loading the salt onto a graphene oxide (GO) surface. The two groups of materials before and after loading were characterized and used as catalysts for the extraction of oxidative organic sulfides in fuel oils. By contrast, the supported catalyst shows better performance. Then, a response surface methodology was used to analyze the influence of reaction conditions on the removal of thiophene and explore the optimum conditions. In addition, the maximum sulfur removal efficiency of T, BT and DBT can reach up to 98.32, 99.98 and 99.28%, respectively. In addition, the catalyst can be easily recovered and reused without any significant decrease in the activity even after ten cycles. This journal is
- Gao, Ruimin,Gao, Yan,Hu, Guangfa,Liu, Zhe,Yang, Lilong,Zhao, Jianshe
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p. 756 - 766
(2022/01/22)
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- Ionic liquid polymer materials with tunable nanopores controlled by surfactant aggregates: A novel approach for CO2capture
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Monomeric ionic liquids (ILs), ionic liquid polymers (ILPs) and IL-based composites have emerged as potential materials for CO2 capture owing to their exceptional intrinsic physical solubility of CO2. This study reports the development of novel IL polymer materials incorporating CO2-philic tunable nanopores and their subsequent utilization for CO2 capture. In this approach, primarily, micelles were formed in monomeric IL 1-vinyl-3-ethylimidazolium bis(trifluoromethylsulfonyl)imide using a CO2-philic surfactant (N-ethyl perfluorooctyl sulfonamide) through self-assembly, from which polymeric materials were fabricated via free radical polymerization. The CO2 adsorption studies demonstrated 3-fold enhancements for the surfactant micelle incorporated IL polymers (SMI-ILPs) compared to their bare IL polymers. The SMI-ILPs were regenerated by simply heating at 70 °C and reused for 15 cycles with a retention of over 96% of CO2 uptake capacity. The simple recovery and notable enhancements in CO2 sorption of novel SMI-ILPs were traced to the adsorption of CO2 at the (i) highly porous IL-based polymeric networks, and (ii) nanometer sized apolar pores made by CO2-philic surfactant tails. This work will open up new possibilities for the development of IL based smart materials for CO2 capture and separation. This journal is
- Bhaskar Reddy, Ambavaram Vijaya,Bustam, Mohamad A.,Goto, Masahiro,Janiak, Christoph,Moniruzzaman, Muhammad,Saha, Bidyut B.
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p. 15034 - 15041
(2020/11/02)
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- Synthesis of Iron(0) Complexes Bearing Protic NHC Ligands: Synthesis and Catalytic Activity
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Preparation of iron(0) pNHC complexes by oxidative addition of N-phosphine-tethered azoles to [Fe3(CO)12] is described. Phosphine-tethered imidazoles 1 and 2 react with [Fe3(CO)12] to give mononuclear iron(0) co
- Mühlen, Christoph,Linde, Jenny,Rakers, Lena,Tan, Tristan T. Y.,Kampert, Florian,Glorius, Frank,Hahn, F. Ekkehardt
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supporting information
p. 2417 - 2421
(2019/07/02)
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- Composite photoanode catalytic system of/CNT (carbon nano /tube) polymer ionic liquid copper complex and application of composite photo-anode catalytic system
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The invention discloses a carbon nano tube/polymerized ionic liquid/copper complex compound light anode catalytic system and application thereof. Polymerized ionic liquid is used for modifying the surfaces of carbon nano tubes noncovalently, copper comple
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Paragraph 0041; 0051-0054
(2019/12/09)
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- Method for water-phase catalysis of Henry asymmetric addition reaction based on polyion liquid type chiral amino acid copper catalyst
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The invention relates to the field of asymmetric catalysis, in particular to a method for water-phase catalysis of a Henry asymmetric addition reaction through a polyion liquid type chiral amino acidcopper catalyst. In a water phase, an aldehyde compound
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Paragraph 0065; 0067-0071
(2019/12/25)
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- Thermally responsive reduced graphene oxide with designable secondary functionality
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Both dual responsive and thermal responsive reduced graphene oxide (rGO) with a strategically inbuilt function have been successfully synthesized by utilizing non-covalent modified poly(NIPAm-co-ViEtImBr) combined with anion exchange.
- Zhang, Qian,Zhang, Junhui,Liu, Bing,Zhang, Ling,Dong, Li,Li, Erni,Zhang, Hairan,Xia, Lixin
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supporting information
p. 6367 - 6370
(2017/07/11)
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- Rationally tuning host-guest interactions to free hydroxide ions within intertrimerically cuprophilic metal-organic frameworks for high OH- conductivity
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Hydroxide-anion-exchange membrane fuel cells (HEMFCs) are now considered as one of the most promising green energy-conversion technologies for stationary and mobile applications, showing high fuel conversion efficiency at high pH and low cost due to their ability to operate under basic conditions using non-precious metal catalysts. But one key impediment to commercialization is insufficient hydroxide ion (OH-) conductivity of the central HEM component. Here, we report the development of free OH- anion-containing metal-organic frameworks (FOMOFs) with rationally tunable host-guest interactions for HEMs with high OH- conductivity. Among three solids obtained by post-synthesis treatment of ultrastable MOF FJU-66 with various bases, free OH- anions are observed in FJU-66·[EVIm]OH with strong host-guest interactions between the MOF backbone and guest cations. Despite the lowest OH- concentration, FJU-66·[EVIm]OH exhibits the highest OH- conductivity close to 0.1 S cm-1. The high OH- conductivity achieved suggests the potential application of the FOMOFs for practical HEMs of fuel cells.
- Li, Ziyin,Zhang, Zhangjing,Ye, Yingxiang,Cai, Kaicong,Du, Fenfen,Zeng, Heng,Tao, Jin,Lin, Quanjie,Zheng, Ying,Xiang, Shengchang
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supporting information
p. 7816 - 7824
(2017/07/15)
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- Polyelectrolyte-catalyzed Diels–Alder reactions
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Imidazolium-based poly(ionic liquids) bearing bromide and bis(trifluoromethane)sulfonimide as counteranions [poly(ViEIm)Br and poly(ViEIm)NTf2] derived from reversible addition fragmentation chain transfer (RAFT) polymerization techniques are u
- Pothanagandhi, Nellepalli,Sivaramakrishna, Akella,Vijayakrishna, Kari
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p. 132 - 136
(2016/08/05)
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- Heterogeneous conversion of CO2 into cyclic carbonates at ambient pressure catalyzed by ionothermal-derived meso-macroporous hierarchical poly(ionic liquid)s
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Meso-macroporous hierarchical poly(ionic liquid)s (MPILs) with extremely high ionic site densities and tunable pore structures were ionothermally synthesized through the free radical self-polymerization of our newly designed rigid bis-vinylimidazolium salt monomer. The synthesis avoided the use of any templates, gave a high yield (>99%) and allowed recycling of the IL solvent; thus it is facile, atom-efficient, environmentally friendly and sustainable. The synthesized MPILs possessed distinctive features of polycation matrices, abundant halogen anions, and large surface areas. They not only presented enhanced CO2 capture, but led to breakthroughs in the heterogeneous catalytic conversion of CO2 into cyclic carbonates: (1) unprecedented high activity at atmospheric pressure and low temperature; (2) good substrate compatibility, even being active towards the extremely inert aliphatic long carbon-chain alkyl epoxides. This result renders the first occasion of a metal-solvent-additive free recyclable heterogeneous cycloaddition of CO2 at such mild conditions.
- Wang, Xiaochen,Zhou, Yu,Guo, Zengjing,Chen, Guojian,Li, Jing,Shi, Yuming,Liu, Yangqing,Wang, Jun
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p. 6916 - 6924
(2015/11/23)
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- Gold immobilized onto poly(ionic liquid) functionalized magnetic nanoparticles: A robust magnetically recoverable catalyst for the synthesis of propargylamine in water
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Supported gold(III) on poly(ionic liquid) coated on magnetic nanoparticles produced a highly active, stable, recoverable and high loading for the synthesis of propargylamines (A3 coupling reaction) under green conditions. The reaction of aldehy
- Moghaddam, Firouz Matloubi,Ayati, Seyed Ebrahim,Hosseini, Seyed Hassan,Pourjavadi, Ali
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p. 34502 - 34510
(2015/04/27)
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- Activated CO2 sorption in mesoporous imidazolium-type poly(ionic liquid)-based polyampholytes
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In this contribution, we present the formation of mesoporous polyampholyte networks via self-complexation (inter-and intrapolyelectrolyte complexation) of copolymers bearing both the imidazolium cations and the carboxylic acid units. The copolymers were p
- Soll, Sebastian,Zhao, Qiang,Weber, Jens,Yuan, Jiayin
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p. 3003 - 3010
(2013/09/02)
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- Poly(basic ionic liquid) coated magnetic nanoparticles: High-loaded supported basic ionic liquid catalyst
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A novel poly(ionic liquid) (PIL) coated magnetic nanoparticle was synthesized by distillation-precipitation-polymerization of 1-vinyl-3- ethyl imidazolium in the presence of surface modified magnetic nanoparticles. The resulting catalyst was used as magne
- Pourjavadi, Ali,Hosseini, Seyed Hassan,AghayeeMeibody, Seyyed Alireza,Hosseini, Seyedeh Talieh
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p. 906 - 911
(2013/10/22)
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- Ionic-liquid-like copolymer stabilized nanocatalysts in ionic liquids: II. Rhodium-catalyzed hydrogenation of arenes
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Rhodium nanoparticles stabilized by the ionic-liquid-like copolymer poly[(N-vinyl-2-pyrrolidone)-co-(1-vinyl-3-butylimidazolium chloride)] were used to catalyze the hydrogenation of benzene and other arenes in ILs. The nanoparticle catalysts can endure forcing conditions (75 °C, 40 bar H2), resulting in high reaction rates and high conversions compared with other nanoparticles that operate in ILs. The hydrogenation of benzene attained record total turnovers of 20,000, and the products were easily separated without being contaminated by the catalysts. Other substrates, including alkyl-substituted arenes, phenol, 4-n-propylphenol, 4-methoxylphenol, and phenyl-methanol, were studied and in most cases were found to afford partially hydrogenated products in addition to cyclohexanes. In-depth investigations on reaction optimization, including characterization of copolymers, transmission electron microscopy, and an infrared spectroscopic study of nanocatalysts, were also undertaken.
- Zhao, Chen,Wang, Han-zhi,Yan, Ning,Xiao, Chao-xian,Mu, Xin-dong,Dyson, Paul J.,Kou, Yuan
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