Co-reporter:Yi Zhang, Xu Zhao, Qiwei Yang, Zhiguo Zhang, Qilong Ren, and Huabin Xing
Industrial & Engineering Chemistry Research June 28, 2017 Volume 56(Issue 25) pp:7336-7336
Publication Date(Web):May 15, 2017
DOI:10.1021/acs.iecr.7b00660
Ionic liquids (ILs) have been proposed as promising solvents for hydrocarbon separations, but designing an industrially attractive IL combining high solubility and low viscosity remains challenging. Here, we synthesized three new long-chain carboxylate ILs with asymmetric phosphonium cations that had relatively low viscosity and good thermal stability and exhibited very high solubility and excellent selectivity for hydrocarbons with different carbon numbers under ambient conditions. The solubilities of propane, ethane, methane, and nitrogen in these tributylethyl-phosphonium long-chain carboxylate ILs were determined at temperatures of 298.1 to 313.1 K and pressures of 20 to 150 kPa. The effects of molecular structure on the properties of ILs and their absorption performance were investigated. It was found that the introduction of an asymmetric cation with short alkyl chains significantly reduced the viscosity of carboxylate ILs, while an extension on the alkyl chain of carboxylate anions enhanced the solubility. At 298.1 K and 150 kPa, the solubilities of propane, ethane, and methane in tributylethylphosphonium stearate reach 0.408, 0.133, and 0.029 mmol/g with selectivities of propane/methane and methane/nitrogen up to 16.92 and 2.72, respectively. This study demonstrates the great potential of long-chain carboxylate ILs as novel solvents for separating light hydrocarbons.
Co-reporter:Xian Suo;Ling Xia;Qiwei Yang;Zhiguo Zhang;Zongbi Bao;Qilong Ren;Yiwen Yang
Journal of Materials Chemistry A 2017 vol. 5(Issue 27) pp:14114-14123
Publication Date(Web):2017/07/11
DOI:10.1039/C7TA01986F
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; Sβ&γ/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.
Co-reporter:Weida Shan;Pengfei Zhang;Shize Yang;Huiyuan Zhu;Peiwen Wu;Sheng Dai
Journal of Materials Chemistry A 2017 vol. 5(Issue 45) pp:23446-23452
Publication Date(Web):2017/11/21
DOI:10.1039/C7TA08994E
A simple, solvent-free, solid-state self-assembly strategy for the synthesis of alkaline-metal-oxide-doped mesoporous carbons (MCs) with tunable mesopores (∼5–9 nm), high surface areas (up to 571 m2 g−1) and large pore volumes (up to 0.65 cm3 g−1) is developed via mechanochemical assembly between polyphenol–Ca2+/Mg2+ composites and F127 copolymers. Interestingly, the as-made MgO-MCs not only offer good CO2 capacities (up to 1.6 mmol g−1 at 0.15 bar and 273 K) and competitive CO2/N2 selectivities (up to 41) but also exhibit high dye adsorption capacities (541 mg g−1 for methylene blue and 435 mg g−1 for methyl orange).
Co-reporter:Xili Cui;Qiwei Yang;Yijun Xiong;Zongbi Bao;Sheng Dai
Chemical Communications 2017 vol. 53(Issue 36) pp:4915-4918
Publication Date(Web):2017/05/02
DOI:10.1039/C7CC01000A
Here we report a facile and effective strategy for the preparation of ordered mesoporous carbon materials with a high-nitrogen-content (8.1 at%) coating layer through a polymer–ionic liquid assembly strategy. The prepared N-doped mesoporous carbon materials demonstrated enhanced CO2 adsorption capacity (2.29 mmol g−1) compared with non-doped carbon (1.84 mmol g−1).
Co-reporter:Xili Cui;Qiwei Yang;Lifeng Yang;Rajamani Krishna;Zhiguo Zhang;Zongbi Bao;Hui Wu;Qilong Ren;Wei Zhou;Banglin Chen
Advanced Materials 2017 Volume 29(Issue 28) pp:
Publication Date(Web):2017/07/01
DOI:10.1002/adma.201606929
The efficient capture of SO2 is of great significance in gas-purification processes including flue-gas desulfurization and natural-gas purification, but the design of porous materials with high adsorption capacity and selectivity of SO2 remains very challenging. Herein, the selective recognition and dense packing of SO2 clusters through multiple synergistic host–guest and guest–guest interactions by controlling the pore chemistry and size in inorganic anion (SiF62−, SIFSIX) pillared metal–organic frameworks is reported. The binding sites of anions and aromatic rings in SIFSIX materials grasp every atom of SO2 firmly via Sδ+···Fδ− electrostatic interactions and Oδ−···Hδ+ dipole–dipole interactions, while the guest–guest interactions between SO2 molecules further promote gas trapping within the pore space, which is elucidated by first-principles density functional theory calculations and powder X-ray diffraction experiments. These interactions afford new benchmarks for the highly efficient removal of SO2 from other gases, even if at a very low SO2 concentration. Exceptionally high SO2 capacity of 11.01 mmol g−1 is achieved at atmosphere pressure by SIFSIX-1-Cu, and unprecedented low-pressure SO2 capacity is obtained in SIFSIX-2-Cu-i (4.16 mmol g−1 SO2 at 0.01 bar and 2.31 mmol g−1 at 0.002 bar). More importantly, record SO2/CO2 selectivity (86–89) and excellent SO2/N2 selectivity (1285–3145) are also achieved. Experimental breakthrough curves further demonstrate the excellent performance of these hybrid porous materials in removing low-concentration SO2.
Co-reporter:Bin Li;Xili Cui;Daniel O'Nolan;Hui-Min Wen;Mengdie Jiang;Rajamani Krishna;Hui Wu;Rui-Biao Lin;Yu-Sheng Chen;Daqiang Yuan;Wei Zhou;Qilong Ren;Guodong Qian;Michael J. Zaworotko;Banglin Chen
Advanced Materials 2017 Volume 29(Issue 47) pp:
Publication Date(Web):2017/12/01
DOI:10.1002/adma.201704210
AbstractRealization of ideal molecular sieves, in which the larger gas molecules are completely blocked without sacrificing high adsorption capacities of the preferred smaller gas molecules, can significantly reduce energy costs for gas separation and purification and thus facilitate a possible technological transformation from the traditional energy-intensive cryogenic distillation to the energy-efficient, adsorbent-based separation and purification in the future. Although extensive research endeavors are pursued to target ideal molecular sieves among diverse porous materials, over the past several decades, ideal molecular sieves for the separation and purification of light hydrocarbons are rarely realized. Herein, an ideal porous material, SIFSIX-14-Cu-i (also termed as UTSA-200), is reported with ultrafine tuning of pore size (3.4 Å) to effectively block ethylene (C2H4) molecules but to take up a record-high amount of acetylene (C2H2, 58 cm3 cm−3 under 0.01 bar and 298 K). The material therefore sets up new benchmarks for both the adsorption capacity and selectivity, and thus provides a record purification capacity for the removal of trace C2H2 from C2H4 with 1.18 mmol g−1 C2H2 uptake capacity from a 1/99 C2H2/C2H4 mixture to produce 99.9999% pure C2H4 (much higher than the acceptable purity of 99.996% for polymer-grade C2H4), as demonstrated by experimental breakthrough curves.
Co-reporter:Zhaoqiang Zhang;Dr. Qiwei Yang;Dr. Xili Cui;Lifeng Yang;Dr. Zongbi Bao; Qilong Ren; Huabin Xing
Angewandte Chemie 2017 Volume 129(Issue 51) pp:16310-16310
Publication Date(Web):2017/12/18
DOI:10.1002/ange.201711715
Das Sortieren von C4-Olefinen gelingt mithilfe einer Kombination aus molekularer Erkennung und Größensiebeffekt. In ihrer Zuschrift auf S. 16500 berichten H. B. Xing und Mitarbeiter über verzahnte poröse Hybridmaterialien mit anionischen Säulen, funktionellen Zentren (die Seerosen) und Hohlräumen (die Durchfahrt unter der Brücke), deren Größe in 0.2-Å-Schritten fein einstellbar ist. Die Materialien ermöglichen eine hervorragende Trennung von C4-Olefinen.
Co-reporter:Zhaoqiang Zhang;Dr. Qiwei Yang;Dr. Xili Cui;Lifeng Yang;Dr. Zongbi Bao; Qilong Ren; Huabin Xing
Angewandte Chemie International Edition 2017 Volume 56(Issue 51) pp:16094-16094
Publication Date(Web):2017/12/18
DOI:10.1002/anie.201711715
The sorting of C4 olefins is possible with a combination of molecular recognition and size-sieving effects. In their Communication on page 16282 ff. H. B. Xing and co-workers report anion-pillared hybrid interpenetrated porous materials with finely tuned cavities (the bridge tunnel) and functional sites (flowers) arranged at 0.2 Å increments. These materials exhibit outstanding performance for the separation of C4 olefins.
Co-reporter:Zhaoqiang Zhang;Dr. Qiwei Yang;Dr. Xili Cui;Lifeng Yang;Dr. Zongbi Bao; Qilong Ren; Huabin Xing
Angewandte Chemie International Edition 2017 Volume 56(Issue 51) pp:16282-16287
Publication Date(Web):2017/12/18
DOI:10.1002/anie.201708769
AbstractC4 olefin separations present one of the great challenges in hydrocarbon purifications owing to their similar structures, thus a single separation mechanism often met with limited success. Herein we report a series of anion-pillared interpenetrated copper coordination for which the cavity and functional site disposition can be varied in 0.2 Å scale increments by altering the anion pillars and organic linkers (GeFSIX-2-Cu-i (ZU-32), NbFSIX-2-Cu-i (ZU-52), GeFSIX-14-Cu-i (ZU-33)), which enable selective recognition of different C4 olefins. In these materials the rotation of the organic linkers is controlled to create a contracted flexible pore window that enables the size-exclusion of specific C4 olefins, while still adsorbing significant amounts of 1,3-butadiene (C4H6) or 1-butene (n-C4H8). Combining the molecular recognition and size-sieving effect, these materials unexpectedly realized the sieving of C4H6/n-C4H8, C4H6/iso-C4H8, and n-C4H8/iso-C4H8 with high capacity.
Co-reporter:Zhaoqiang Zhang;Dr. Qiwei Yang;Dr. Xili Cui;Lifeng Yang;Dr. Zongbi Bao; Qilong Ren; Huabin Xing
Angewandte Chemie 2017 Volume 129(Issue 51) pp:16500-16505
Publication Date(Web):2017/12/18
DOI:10.1002/ange.201708769
AbstractC4 olefin separations present one of the great challenges in hydrocarbon purifications owing to their similar structures, thus a single separation mechanism often met with limited success. Herein we report a series of anion-pillared interpenetrated copper coordination for which the cavity and functional site disposition can be varied in 0.2 Å scale increments by altering the anion pillars and organic linkers (GeFSIX-2-Cu-i (ZU-32), NbFSIX-2-Cu-i (ZU-52), GeFSIX-14-Cu-i (ZU-33)), which enable selective recognition of different C4 olefins. In these materials the rotation of the organic linkers is controlled to create a contracted flexible pore window that enables the size-exclusion of specific C4 olefins, while still adsorbing significant amounts of 1,3-butadiene (C4H6) or 1-butene (n-C4H8). Combining the molecular recognition and size-sieving effect, these materials unexpectedly realized the sieving of C4H6/n-C4H8, C4H6/iso-C4H8, and n-C4H8/iso-C4H8 with high capacity.
Co-reporter:Wenbin Jin, Qiwei Yang, Binbin Huang, Zongbi Bao, Baogen Su, Qilong Ren, Yiwen Yang and Huabin Xing
Green Chemistry 2016 vol. 18(Issue 12) pp:3549-3557
Publication Date(Web):26 Apr 2016
DOI:10.1039/C6GC00584E
Water is an ideal green solvent for the solubilization and separation of valued-added bioactive compounds in various chemical and biological processes, partly because water has a minimal impact on the environment and few safety issues. However, many bioactive compounds exhibit hydrophobic properties, which leads to their limited solubility in water and substantially hinders the development of green separation technologies using aqueous media. In this study, we construct a family of new water/ionic liquid (IL) mixtures with amphiphilic, anionic functional long-chain carboxylate ionic liquids (LCC-ILs) for the solubilization and extraction of hydrophobic bioactive compounds (HBCs). The LCC-ILs integrate both weak polarity and strong hydrogen-bonding basicity and, more importantly, have excellent lipophilicity while still being water-miscible; therefore, the water/LCC-IL mixtures exhibit extremely high solubilities for various HBCs. The quantitative solubilities (g g−1) of various HBCs, including tocopherol, perillyl alcohol, rutin, and ginkgolides, are as high as 1.46, 0.71, 0.39 and 0.43, respectively, at 35 °C in water/LCC-IL mixtures, which are the highest solubilities in aqueous solutions ever reported. The water/LCC-IL mixtures also exhibit excellent performance in the extraction of tocopherols from biomass with a yield 2 to 12 times that in common solvents. The microscopic solvent properties and dissolution mechanism were investigated. Nano-micelles were observed when tocopherol was dissolved in water/LCC-IL mixtures, and their dissolution ability was dependent on the alkyl chain length and the concentration of LCC-ILs. These results demonstrated the considerable potential of water/LCC-IL mixtures as promising green solvents for the solubilization and separation of HBCs.
Co-reporter:Zhenkang Li, Zhiping Wang, Qiwei Yang, Zhiguo Zhang, Yiwen Yang, Qilong Ren, and Huabin Xing
ACS Sustainable Chemistry & Engineering 2016 Volume 4(Issue 8) pp:4403
Publication Date(Web):July 5, 2016
DOI:10.1021/acssuschemeng.6b00997
Ionic liquid (IL)-mediated extraction methods have drawn much attention due to their reduced environmental impact and improved extraction efficiencies compared to traditional separation methods. However, one long-standing challenge in the application of IL-based extraction processes is the difficulty in recovering high-boiling solutes from the IL phase due to the negligible vapor pressure of ILs and the strong interaction between solutes and ILs. In this study, a new CO2-assisted back-extraction method was developed for the recovery of high-boiling solutes from the IL phase based on the reversible chemical absorption and/or strong physical interaction of CO2 with ILs. We found the distribution coefficient (D) of the typical solute δ-tocopherol in the [P4444][Pro]/DMSO–hexane biphasic system significantly decreased from 10.38 to 2.42 after the introduction of CO2, which greatly reduced the required solvent consumption and the number of back-extractions required for tocopherol recovery. For example, the number of back-extractions required for the recovery of 90% of the tocopherols from the [P4444][Pro]/DMSO–hexane biphasic phase decreased from 24 to 5 with the aid of CO2 absorption, along with a decrease in solvent consumption by approximately 80%. The effects of the structure of the IL, the loading of CO2, the type of cosolvents, and the temperature of the CO2-assisted back-extraction processes were investigated in this study. This proof-of-concept study demonstrates the great potential of CO2-assisted back-extraction as a green method for the efficient recovery of high-boiling solutes from the IL phase.Keywords: Back-extraction; Bioactive compounds; Carbon dioxide; Extraction; Ionic liquids
Co-reporter:Dr. Qiwei Yang;Zhiping Wang;Dr. Zongbi Bao;Dr. Zhiguo Zhang; Yiwen Yang; Qilong Ren; Huabin Xing; Sheng Dai
ChemSusChem 2016 Volume 9( Issue 8) pp:
Publication Date(Web):
DOI:10.1002/cssc.201600428
Co-reporter:Dr. Qiwei Yang;Zhiping Wang;Dr. Zongbi Bao;Dr. Zhiguo Zhang; Yiwen Yang; Qilong Ren; Huabin Xing; Sheng Dai
ChemSusChem 2016 Volume 9( Issue 8) pp:
Publication Date(Web):
DOI:10.1002/cssc.201600429
Abstract
Invited for this month′s cover is the group of Huabin Xing at Zhejiang University. The image depicts the dominance of a 1:1 reaction mechanism for CO2 capture using a proline-based ionic liquid. The Full Paper itself is available at 10.1002/cssc.201501691.
Co-reporter:Dr. Qiwei Yang;Zhiping Wang;Dr. Zongbi Bao;Dr. Zhiguo Zhang; Yiwen Yang; Qilong Ren; Huabin Xing; Sheng Dai
ChemSusChem 2016 Volume 9( Issue 8) pp:806-812
Publication Date(Web):
DOI:10.1002/cssc.201501691
Abstract
The last decade saw an explosion of interest in using amine-functionalized materials for CO2 capture and conversion, and it is of great importance to elucidate the relationship between the molecular structure of amine-functionalized materials and their CO2 capacity. In this work, based on a new quantitative analysis method for the CO2 absorption mechanism of amino-acid ionic liquids (ILs) and quantum chemical calculations, we show that the small difference in the local structure of amine groups in ILs could lead to much different CO2 absorption mechanisms, which provides an opportunity for achieving higher CO2 capacity by structure design. This work revealed that the actual CO2 absorption mechanism by amino-acid ILs goes beyond the apparent CO2/amine stoichiometry; a rigid ring structure around the amine group in ILs creates a unique electrostatic environment that inhibits the deprotonation of carbamic acid and enables actually equimolar CO2/amine absorption.
Co-reporter:Xili Cui;Kaijie Chen;Qiwei Yang;Rajamani Krishna;Zongbi Bao;Hui Wu;Wei Zhou;Xinglong Dong;Yu Han;Bin Li;Qilong Ren;Michael J. Zaworotko;Banglin Chen
Science 2016 Volume 353(Issue 6295) pp:141-144
Publication Date(Web):08 Jul 2016
DOI:10.1126/science.aaf2458
Separating one organic from another
Separating closely related organic molecules is a challenge (see the Perspective by Lin).The separation of acetylene from ethylene is needed in high-purity polymer production. Cui et al. developed a copper-based metal-organic framework with hexafluorosilicate and organic linkers designed to have a high affinity for acetylene. These materials, which capture four acetylene molecules in each pore, successfully separated acetylene from mixtures with ethylene. Propane and propylene are both important feedstock chemicals. Their physical and chemical similarity, however, requires energy-intense processes to separate them. Cadiau et al. designed a fluorinated porous metal-organic framework material that selectively adsorbed propylene, with the complete exclusion of propane.
Science, this issue pp. 141 and 137; see also p. 121
Co-reporter:Jingyi Hu, Qiwei Yang, Lifeng Yang, Zhiguo Zhang, Baogen Su, Zongbi Bao, Qilong Ren, Huabin Xing, and Sheng Dai
ACS Catalysis 2015 Volume 5(Issue 11) pp:6724
Publication Date(Web):October 1, 2015
DOI:10.1021/acscatal.5b01690
Metal catalysts often encounter the dilemma of rapid deactivation due to reduction or particle aggregation/growth during the reaction. Here we reported an active and stable metal nanoparticles (NPs)/surfactant ionic liquid (IL) system for the catalytic hydrochlorination of acetylene. The NPs of Pd, Au, and Pt with a narrow size distribution and well-defined lattice fringes experienced in situ generation in the reaction medium of anionic surfactant carboxylate ILs (ASC-ILs). Benefiting from the high reactivity of NPs and the self-assembly property of ASC-ILs, an effective redox cycle between Pd0 and PdII was established to reduce the deactivation of metal catalysts. The Pd NPs/surfactant IL systems showed excellent catalytic activity toward acetylene hydrochlorination. An acetylene conversion of 93% and a selectivity of 99.5% were achieved with no discernible deterioration over a reaction time of 55 h. Furthermore, ASC-ILs were endowed with a unique property of the strong hydrogen-bond basicity, which was effective in absorbing and activating acetylene and HCl. This study manifests that metal NPs/surfactant IL systems are promising as substitutes for toxic mercury catalysts in the hydrochlorination of acetylene, and also is instructive for the stabilization of metal NPs.Keywords: acetylene; hydrochlorination; ionic liquid; nanoparticles; nonmercuric; palladium
Co-reporter:Wenbin Jin, Qiwei Yang, Zhiguo Zhang, Zongbi Bao, Qilong Ren, Yiwen Yang and Huabin Xing
Chemical Communications 2015 vol. 51(Issue 67) pp:13170-13173
Publication Date(Web):01 Jul 2015
DOI:10.1039/C5CC03463A
Here we report a novel self-assembly induced solubilization strategy with nanostructured ionic liquids as solvents. Highly ordered mesoscopic structures featuring the solute as a key component, such as liquid crystals, were formed via self-assembly in nanostructured long-chain carboxylate ionic liquids, resulting in extremely high solubilities for sparingly soluble drug molecules.
Co-reporter:Yuanbang Xie, Huabin Xing, Qiwei Yang, Zongbi Bao, Baogen Su, and Qilong Ren
ACS Sustainable Chemistry & Engineering 2015 Volume 3(Issue 12) pp:3365
Publication Date(Web):October 26, 2015
DOI:10.1021/acssuschemeng.5b01068
Ionic liquid-based aqueous biphasic systems (IL-based ABSs) offer a benign alternative process for conventional extraction systems with volatile organic solvents to separate biomass. Designing an IL-based ABS with excellent phase splitting ability, remarkable extraction efficiency, and good biocompatibility remains challenging. In this work, we report a series of novel ABSs using biocompatible ILs composed of long chain carboxylate anions and a cholinium cation that are all derived from biomass. This strategy introduced long alkyl chains into the anions, which not only significantly increased the hydrogen bond (HB) acceptor ability of the carboxylate anions through a remarkable electron-donating effect but also ensured good hydrophobicity for achieving better phase splitting. The developed IL-based ABS demonstrated a relatively broad biphasic area and extraordinary extraction efficiency for amino acids and bioactive compounds with distribution coefficients for tryptophan, phenylalanine, and caffeine of 58.5, 120 (120 was set as a maximum value for the partition coefficient because in some cases the concentration of the extracted material in the salt-rich phase was below the limit of detection), and 120, respectively, which were remarkably higher than those obtained in ABS with conventional ILs. This work shows that the long chain carboxylate anion is critical for the excellent extraction performance of the developed ABS and that their distribution coefficients increased with increasing anion alkyl chain lengths. In addition, liquid crystal structures were observed when the carbon number of the carboxylate anion of the ILs exceeded eight; thus, IL-based ABS with liquid crystal structures were reported for the first time.Keywords: Aqueous biphasic system; Extraction; Hydrogen bond; Ionic liquids; Liquid crystal
Co-reporter:Qiwei Yang, Dan Xu, Jingzhu Zhang, Yaoming Zhu, Zhiguo Zhang, Chao Qian, Qilong Ren, and Huabin Xing
ACS Sustainable Chemistry & Engineering 2015 Volume 3(Issue 2) pp:309
Publication Date(Web):December 15, 2014
DOI:10.1021/sc5006796
The development of ionic liquids (ILs) with strong hydrogen-bond basicity is of great importance for the application of ILs in liquid–liquid extractions, but a long-standing problem is that the increase in hydrogen-bond basicity of ILs usually comes along with undesired changes in other properties such as reduced lipophilicity, raised melting point, and difficulty of forming biphasic systems with water. Herein, we provided a promising solution to this problem by synthesizing a class of functional phosphonium ILs with the use of biocompatible saturated/unsaturated long-chain fatty acids (carbon number up to 20) as anion precursors, and we also carried out systematic investigations on their physicochemical properties. These long-chain fatty acid ILs (LCFA-ILs) featured very strong hydrogen-bond basicity, up to the top level of all reported solvents, along with good lipophilicity and a wide liquid range. Moreover, the viscosity of LCFA-ILs exhibited only a slight increase with increasing chain length, and the hydrophilicity/hydrophobicity could be tuned by a change in the side chain of the phosphonium cation. Excellent extraction efficiency was achieved by applying LCFA-ILs to both aqueous and nonaqueous extractions. The distribution coefficients of specific solutes reached unprecedented values up to 3000–5000, which were 17–650 times higher than those by common ILs and molecular solvents.Keywords: Basicity; Extraction; Hydrogen bond; Ionic liquid; Phenol; Solvatochromic
Co-reporter:Jingzhu Zhang, Kun Yu, Qiwei Yang, Zongbi Bao, Zhiguo Zhang, Yiwen Yang, Qilong Ren and Huabin Xing
RSC Advances 2015 vol. 5(Issue 95) pp:77581-77588
Publication Date(Web):07 Sep 2015
DOI:10.1039/C5RA14202D
Natural zwitterionic compounds are widely used as surfactants, drugs and food additives. However, obtaining high-purity zwitterions from biomass remains challenging because of the presence of structurally similar homologues in plants. Here, we developed a novel extraction method to separate zwitterionic phospholipid homologues using ionic liquids (ILs) as extractants. A large distribution coefficient and excellent separation selectivity for phosphatidylcholine (PC) were achieved with hydroxyl-functionalized and carboxyl-functionalized ILs as the extractants. An effective IL–cosolvent extraction strategy was employed in this work to reduce the consumption of IL and improve the extraction efficiency. Additionally, the underlying extraction mechanism was explored using ab initio calculations and dynamic light scattering. The results indicated the existence of multiple hydrogen-bonding interactions between the IL and both the negative and positive moieties of the zwitterion, and the formation of micelles in the IL–cosolvent mixture was also observed. In addition, the effects of the structure and concentration of ILs and the temperature on extraction performance were investigated, and the feasibility of recovery of ILs by electrodialysis was evaluated.
Co-reporter:Xianxian Liu;Dr. Qiwei Yang;Dr. Zongbi Bao;Dr. Baogen Su;Dr. Zhiguo Zhang; Qilong Ren; Yiwen Yang ; Huabin Xing
Chemistry - A European Journal 2015 Volume 21( Issue 25) pp:9150-9156
Publication Date(Web):
DOI:10.1002/chem.201500306
Abstract
A class of new ionic liquid (IL)-based nonaqueous lyotropic liquid crystals (LLCs) and the development of an efficient IL extraction process based on LC chemistry are reported. The nonaqueous LLCs feature extraordinarily high extraction capacity, excellent separation selectivity, easy recovery, and biocompatibility. This work also demonstrates that the introduction of self-assembled anisotropic nanostructures into an IL system is an efficient way to overcome the intrinsically strong polarity of ILs and enhances the molecular recognition ability of ILs. The distribution coefficients of IL-based LLCs for organic compounds with H-bond donors reached unprecedented values of 50–60 at very high feed concentrations (>100 mg mL−1), which are 800–1000 times greater than those of common ILs as well as traditional organic and polymer extractants. The IL-based nonaqueous LLCs combining the unique properties of ILs and LCs open a new avenue for the development of high-performance extraction methods.
Co-reporter:Liyun Kong, Qiwei Yang, Huabin Xing, Baogen Su, Zongbi Bao, Zhiguo Zhang, Yiwen Yang and Qilong Ren
Green Chemistry 2014 vol. 16(Issue 1) pp:102-107
Publication Date(Web):15 Oct 2013
DOI:10.1039/C3GC41804A
A new method for the effective separation of amphiphilic poly(ethylene glycol) mono- and di-esters with long-chain ionic liquid-based biphasic systems has been developed. These biphasic systems exhibited high selectivity, a large distribution coefficient and a good ability to eliminate the emulsification resulting from the surface active character of those amphiphilic molecules.
Co-reporter:Yifeng Cao, Huabin Xing, Qiwei Yang, Zhenkang Li, Ting Chen, Zongbi Bao, and Qilong Ren
Industrial & Engineering Chemistry Research 2014 Volume 53(Issue 26) pp:10784-10790
Publication Date(Web):2017-2-22
DOI:10.1021/ie5007273
The design of a biphasic system is important for the development of liquid–liquid extraction and biphasic catalysis. In this work, we report a series of ternary biphasic systems that consist of hydrophilic ionic liquid (IL), water, and ethyl acetate. The effects of the structure of the ILs (cation, anion, and substituent group), IL/water ratio, and temperature on the phase equilibrium of these biphasic systems were investigated. The mutual solubility was lower in the IL/water–ethyl acetate biphasic system than in the water–ethyl acetate system when ILs with strong hydration ability were introduced, such as [EMIm]OAc, [EMIm]Cl, [EMIm]NO3, [EMIm]EtSO4, and [HOEMIm]Cl. In addition, the hydrogen-bonding basicity of the IL-containing phase could be tuned by changing the IL structure or IL/water ratio. These novel IL/water-ethyl acetate biphasic systems may present another option in addition to hydrophobic IL–water and aqueous biphasic systems for liquid–liquid extraction.
Co-reporter:Qiwei Yang, Huabin Xing, Zongbi Bao, Baogen Su, Zhiguo Zhang, Yiwen Yang, Sheng Dai, and Qilong Ren
The Journal of Physical Chemistry B 2014 Volume 118(Issue 13) pp:3682-3688
Publication Date(Web):March 12, 2014
DOI:10.1021/jp500790r
The basicity of ionic liquids (ILs) underlies many important IL-based processes including the dissolution and conversion of cellulose, the capture of CO2, and metal catalysis. In this work, we have disclosed the nature of the basicity of ILs, i.e., the difference between the basicity of IL and the basicity of the molecular solvent and inorganic salt, through a quantitative electrostatic and electronic analysis of the molecular surface for the first time. The results reveal one of the distinctive properties of ILs (enhanced basicity over molecular solvents and inorganic salts with the same basic site) stemming from their special electrostatic environment and microstructure. The enhancement is significant, from either the electrostatic aspect or the covalent aspect of basicity. The peculiar electrostatic environment of ILs leads to stronger basicity than similar molecular solvents, and the relatively freer microstructure of ILs contributes to the enhancement of basicity over their inorganic analogues. These results are highly instructive for better understanding the unique value of ILs and designing novel ILs to improve the efficiency of basicity-related processes.
Co-reporter:Dan Xu, Qiwei Yang, Baogen Su, Zongbi Bao, Qilong Ren, and Huabin Xing
The Journal of Physical Chemistry B 2014 Volume 118(Issue 4) pp:1071-1079
Publication Date(Web):January 3, 2014
DOI:10.1021/jp4096503
Ionic liquids (ILs) with relatively strong basicity often show impressive performance in chemical processes, so it is important to enhance the basicity of ILs by molecular design. Here, we proposed two effective ways to enhance the basicity of ILs: by weakening the cation–anion interaction strength and by employing the anion-tethered strategy. Notably, two quantum-chemical parameters, the most negative surface electrostatic potential and the lowest surface average local ionization energy, were adopted as powerful tools to demonstrate the electrostatic and covalent aspects of basicity, respectively, at the microscopic level. It was shown that, for the ILs with the same anion (acetate or trifluoroacetate), the basicity of the ILs could be enhanced when the cation–anion interaction strength was weakened. For the acetate anion-based ILs, the hydrogen-bonding basicity scale (β) increased by 29% when the cation changed from 1-butyl-3-methylimidazolium ([Bmim]) to tetrabutylphosphonium ([P4444]), achieving one of the highest reported β values for ILs. Moreover, it was also demonstrated that, when an amine group was tethered to the anion of the IL, its basicity was stronger than when it was tethered to the cation. These results are highly instructive for designing ILs with strong basicity and for improving the efficiency of IL-based processes, such as CO2 capture, SO2 and acetylene absorption, dissolution of cellulose, extraction of bioactive compounds, and so on.
Co-reporter:Dr. Huabin Xing;Dr. Chen Liao;Dr. Qiwei Yang;Dr. Gabriel M. Veith;Dr. Bingkun Guo;Dr. Xiao-Guang Sun; Qilong Ren; Yong-Sheng Hu; Sheng Dai
Angewandte Chemie International Edition 2014 Volume 53( Issue 8) pp:2099-2103
Publication Date(Web):
DOI:10.1002/anie.201309539
Abstract
Li-SO2 batteries have a high energy density but bear serious safety problems that are associated with pressurized SO2 and flammable solvents in the system. Herein, a novel ambient Li-SO2 battery was developed through the introduction of ionic liquid (IL) electrolytes with tailored basicities to solvate SO2 by reversible chemical absorption. By tuning the interactions of ILs with SO2, a high energy density and good discharge performance with operating voltages above 2.8 V were obtained. This strategy based on reversible chemical absorption of SO2 in IL electrolytes enables the development of the next generation of ambient Li-SO2 batteries.
Co-reporter:Dr. Huabin Xing;Dr. Chen Liao;Dr. Qiwei Yang;Dr. Gabriel M. Veith;Dr. Bingkun Guo;Dr. Xiao-Guang Sun; Qilong Ren; Yong-Sheng Hu; Sheng Dai
Angewandte Chemie 2014 Volume 126( Issue 8) pp:2131-2135
Publication Date(Web):
DOI:10.1002/ange.201309539
Abstract
Li-SO2 batteries have a high energy density but bear serious safety problems that are associated with pressurized SO2 and flammable solvents in the system. Herein, a novel ambient Li-SO2 battery was developed through the introduction of ionic liquid (IL) electrolytes with tailored basicities to solvate SO2 by reversible chemical absorption. By tuning the interactions of ILs with SO2, a high energy density and good discharge performance with operating voltages above 2.8 V were obtained. This strategy based on reversible chemical absorption of SO2 in IL electrolytes enables the development of the next generation of ambient Li-SO2 batteries.
Co-reporter:Huabin Xing, Xu Zhao, Rulong Li, Qiwei Yang, Baogen Su, Zongbi Bao, Yiwen Yang, and Qilong Ren
ACS Sustainable Chemistry & Engineering 2013 Volume 1(Issue 11) pp:1357
Publication Date(Web):August 18, 2013
DOI:10.1021/sc400208b
As green and designable solvents, ionic liquids (ILs), have great potential in the separation of olefins and paraffins. The introduction of functional groups into ILs enhances its separation selectivity for olefin to paraffin; however, the absorption capacities of such functionalized ILs obviously decrease due to the strong polarity of the functional group. In this work, we designed a symmetrical dual nitrile-functionalized IL 1,3-dibutyronitrile-imidazolium bis((trifluoromethyl)sulfonyl)imide ([(CP)2im][NTf2]) and determined the solubility of ethylene and ethane at 303.15 K in three ILs: nonfunctionalized 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([Bmim][NTf2]), single-functionalized 1-butyronitrile-3-methylimidazolium bis((trifluoromethyl)sulfonyl)imide ([CPmim][NTf2]), and dual-functionalized [(CP)2im][NTf2]. The experimental results showed that enhanced separation selectivity for ethylene/ethane could be achieved in the symmetrical dual-functionalized [(CP)2im][NTf2] with only a slight reduction of absorption capacity. A COSMO-RS calculation was carried out to understand the underlying dissolution mechanism of ethylene and ethane in ILs and showed that the polarity of the IL and its misfit interaction with gases were the major factors in determining the solubilities of ethylene and ethane in it. In addition, a silver-containing IL was also tested because of its higher absorption capacity for olefins. It was found that the silver-containing IL was superior to any of the common ILs in the separation of ethylene/ethane, particularly [Bmim][NTf2]. A simple equilibrium model was used to describe the absorption of ethylene in the silver-containing IL.Keywords: Absorption; Dual nitrile-functionalized; Ionic liquids; Symmetrical; π-Complexation;
Co-reporter:Huabin Xing, Xu Zhao, Qiwei Yang, Baogen Su, Zongbi Bao, Yiwen Yang, and Qilong Ren
Industrial & Engineering Chemistry Research 2013 Volume 52(Issue 26) pp:9308
Publication Date(Web):June 7, 2013
DOI:10.1021/ie400999f
As environmentally friendly and designable solvents, ionic liquids (ILs) have great potential in the separation of C2H4 and C2H2, which is quite important in chemical industry. The microscopic insight into the intermolecular interaction and the diffusion dynamics at a molecular level is crucial for designing more efficient ILs. In this work, the interaction mechanism and diffusion dynamics for C2H4/C2H2 absorption and separation with five ILs, 1-butyl-3-methylimidazolium tetrafluoroborate ([bmim][BF4]), 1-butyl-3-methylimidazolium acetate ([bmim][OAc]), 1-butyl-3-methylimidazolium trifluoroacetate ([bmim][TFA]), 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([bmim][Tf2N]), and 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([bmpyrr][Tf2N]), were investigated by molecular dynamics (MD) simulation. The result suggests that the van der Waals interaction between C2H4 and cation plays an important role in C2H4 dissolution in ILs, but the hydrogen bonding interaction between C2H2 and anion is foremost in C2H2 dissolution. Moreover, the interaction energy analysis matches better with the experimental solubility than our previous quantum chemical calculation, indicating the superiority of the MD simulation approach in studying the interaction mechanism of IL-based systems where multiple interactions are often present. The self-diffusion coefficients of cations and anions of ILs do not change obviously after adding C2H4, while they have a significant increase after dissolving C2H2, particularly in relatively strong hydrogen bonding systems [bmim][OAc]–C2H2.
Co-reporter:Yifeng Cao, Huabin Xing, Qiwei Yang, Baogen Su, Zongbi Bao, Ruihan Zhang, Yiwen Yang and Qilong Ren
Green Chemistry 2012 vol. 14(Issue 9) pp:2617-2625
Publication Date(Web):11 Jul 2012
DOI:10.1039/C2GC35614G
Separation of high value bioactive compounds is a viable route to make full use of the biomass resources and improve the profitability. However, the sparing aqua- and lipo-solubility of the bioactive compounds makes their separation really challenging. Considering that ionic liquids show good solubility of biomass and could easily form biphasic systems with organic solvents, an ionic liquid (IL)-based biphasic system consisting of ionic liquid, water and ethyl acetate is proposed in this study. Ginkgolide homologues were selected as model compounds to evaluate its practicality. Adequate distribution coefficients, relatively high extraction capacity and selectivity were obtained with the novel biphasic system. The improved distribution coefficients of the ginkgolides are mainly attributed to the multiple interactions between ginkgolide and IL, which were confirmed by means of quantum chemistry calculations. Moreover, the effect of the interactions between ginkgolides and the extraction solvent on the selectivity coefficient was studied by measuring the Kamlet–Taft parameters of the extraction solvent. Based on the results of fractional extraction, which was simulated by calculation and validated by experiments, as well as the comparison of organic solvent consumption, the employed IL-based extraction would be a valid and clean method as an alternative to chromatographic methods for separating bioactive compounds in large-scale operations. It is noteworthy that the amount of organic solvents consumed with this method was supposed to be less than 1/11 of the most widely used chromatographic method.
Co-reporter:Rulong Li, Huabin Xing, Qiwei Yang, Xu Zhao, Baogen Su, Zongbi Bao, Yiwen Yang, and Qilong Ren
Industrial & Engineering Chemistry Research 2012 Volume 51(Issue 25) pp:8588-8597
Publication Date(Web):June 9, 2012
DOI:10.1021/ie3001452
This paper presents an extensive study on the feasibility of ionic liquids (ILs) for the extractive separation of a 1-hexene/n-hexane mixture. Seventeen ILs were tested at 313 K. The extraction selectivities of 1-hexene to n-hexane were in the range 1.5–3.0. The chemical structures of anion and cation in ILs greatly affected the extraction, and the functional groups, such as carbon–carbon double bond, nitrile, ester, and amide, in the ILs led to higher selectivities. The increase of alkyl chain length in cation led to the increase of extraction capacity of 1-hexene. To increase the distribution of 1-hexene in IL phase, silver salt was added to the ILs. It was found that ILs containing silver salt had a high distribution of 1-hexene, as well as high selectivity of 1-hexene against n-hexane. The extraction efficiency increased with the concentration of silver salt in ILs. When the initial feed concentration of 1-hexene was smaller, the selectivity of 1-hexene to n-hexane was higher. A simple mathematical model has been developed to describe the total 1-hexene content in the reaction media under study, on the basis of the formation of complexes between silver and 1-hexene with different stoichiometry. This work proves that the ILs can act as effective extractants in 1-hexene/n-hexane separation.
Co-reporter:Xiaolei Ni, Huabin Xing, Qiwei Yang, Jun Wang, Baogen Su, Zongbi Bao, Yiwen Yang, and Qilong Ren
Industrial & Engineering Chemistry Research 2012 Volume 51(Issue 18) pp:6480-6488
Publication Date(Web):March 27, 2012
DOI:10.1021/ie201682h
Amino acid ionic liquids (AAILs) with different amino acid anions were investigated in the selective separation of a typical natural phenolic product, α-tocoperol, from its mixture with methyl linoleate by liquid–liquid extraction. A large separation selectivity, suitable distribution coefficient, and adequate extraction capacity were achieved with the AAIL/N,N-dimethylformamide (DMF) mixture as extractant. The selectivity of α-tocopherol to methyl linoleate reached up to 29 when using [emim]Ala and [emim]Lys as the extractant diluted by DMF with mole ratio of AAIL to DMF 15:85, at least 9 times larger than that using DMF or common ILs as the extractant. The presence of diluents, DMF, can not only reduce the viscosity of IL phase, but could also lead to much larger distribution coefficients. Back extraction of α-tocopherol using hexane and reuse of AAIL were both tested. Solvatochromic and infrared spectra measurements were used to investigate the mechanism of α-tocopherol extraction with ILs. A close linear relationship can be drawn between the distribution coefficients of α-tocopherol and the hydrogen-bond basicity (β) of the extraction solvents, and also between the selectivites and the β values.
Co-reporter:Yifeng Cao, Huabin Xing, Qiwei Yang, Zongbi Bao, Baogen Su, Yiwen Yang, and Qilong Ren
Journal of Agricultural and Food Chemistry 2012 Volume 60(Issue 13) pp:3432-3440
Publication Date(Web):March 4, 2012
DOI:10.1021/jf3003009
The separation of a compound of interest from its structurally similar homologues is an important and challenging problem in producing high-purity natural products, such as the separation of genistein from other soybean isoflavone aglycone (SIA) homologues. The present work provided a novel method for separating genistein from its structurally similar homologues by ionic liquid (IL)-based liquid–liquid extraction using hydrophobic IL–water or hydrophilic IL/water–ethyl acetate biphasic systems. Factors that influence the distribution equilibrium of SIAs, including the structure and concentration of IL, pH value of the aqueous phase, and temperature, were investigated. Adequate distribution coefficients and selectivities over 7.0 were achieved with hydrophilic IL/water–ethyl acetate biphasic system. Through a laboratory-scale simulation of fractional extraction process containing four extraction stages and four scrubbing stages, genistein was separated from the SIA homologues with a purity of 95.3% and a recovery >90%.
Co-reporter:Xu Zhao, Huabin Xing, Qiwei Yang, Rulong Li, Baogen Su, Zongbi Bao, Yiwen Yang, and Qilong Ren
The Journal of Physical Chemistry B 2012 Volume 116(Issue 13) pp:3944-3953
Publication Date(Web):March 13, 2012
DOI:10.1021/jp211095y
The room-temperature ionic liquids (RTILs) have potential in realizing the ethylene (C2H4) and acetylene (C2H2) separation and avoiding solvent loss and environmental pollution compared with traditional solvents. The interaction mechanisms between gases and RTILs are important for the exploration of new RTILs for gas separation; thus, they were studied by quantum chemical calculation and molecular dynamics simulation in this work. The optimized geometries were obtained for the complexes of C2H4/C2H2 with anions (Tf2N–, BF4–, and OAc–), cation (bmim+), and their ion pairs, and the analysis for geometry, interaction energy, natural bond orbital (NBO), and atoms in molecules (AIM) was performed. The quantum chemical calculation results show that the hydrogen-bonding interaction between the gas molecule and anion is the dominant factor in determining the solubility of C2H2 in RTILs. However, the hydrogen-bonding interaction, the p–π interaction in C2H4–anion, and the π–π interaction in C2H4–cation are weak and comparable, which all affect the solubility of C2H4 in RTILs with comparable contribution. The calculated results for the distance of Hgas···X (X = O or F in anions), the BSSE-corrected interaction energy, the electron density of Hgas···X at the bond critical point (ρBCP), and the relative second-order perturbation stabilization energy (E(2)) are consistent with the experimental data that C2H2 is more soluble than C2H4 in the same RTILs and the solubility of C2H4 in RTILs has the following order: [bmim][Tf2N] > [bmim][OAc] > [bmim][BF4]. The calculated results also agree with the order of C2H2 solubility in different RTILs that [bmim][OAc] > [bmim][BF4] > [bmim][Tf2N]. Furthermore, the calculation results indicate that there is strong C2H2–RTIL interaction, which cannot be negligible compared to the RTIL–RTIL interaction; thus, the regular solution theory is probably not suitable to correlate C2H2 solubility in RTILs. The molecular dynamics simulation results show that the hydrogen bond between the H in C2 of the imidazolium cation and the anion will weaken the hydrogen-bonding interaction of the gas molecule and anion in a realistic solution condition, especially in the C2H4–RTIL system.
Co-reporter:Qiwei Yang, Hai Zhang, Baogen Su, Yiwen Yang, Qilong Ren and Huabin Xing
Journal of Chemical & Engineering Data 2010 Volume 55(Issue 4) pp:1750-1754
Publication Date(Web):January 15, 2010
DOI:10.1021/je900733j
Densities for binary mixtures consisting of 1-butyl-3-methylimidazolium chloride ([bmim]Cl) and water or hydrophilic organic solvents (methanol, acetonitrile, and N,N-dimethylformamide) have been determined at different temperatures ranging from (293.15 to 318.15) K and atmospheric pressure, with mole fractions of [bmim]Cl in the mixtures ranging from 0 to about 0.5. The density values increase as the [bmim]Cl concentration increases or the temperature decreases, and the temperature dependence has been correlated by a second-order polynomial equation. The isobaric expansivity and apparent molar volume values for these binary mixtures have been calculated from the density data. A comparison has been made for the obtained properties with those of similar systems reported in the literature when available.
Co-reporter:Qiwei Yang, Huabin Xing, Yifeng Cao, Baogen Su, Yiwen Yang and Qilong Ren
Industrial & Engineering Chemistry Research 2009 Volume 48(Issue 13) pp:6417-6422
Publication Date(Web):May 27, 2009
DOI:10.1021/ie801847e
Selective separation of tocopherol homologues was performed by liquid−liquid extraction, using ionic liquids (ILs) as extractants in the presence of diluent. The distribution coefficients and selectivities of tocopherols in the biphasic system were determined. A selectivity of δ-tocopherol to α-tocopherol up to 21.3 was achieved when using [bmim]Cl as extractant diluted by methanol. Considering the structural differences of tocopherols, the separation mechanism based on the hydrogen-bonding interaction between IL’s anion and the −OH group on the tocopherols was proposed. The separation efficiency of IL was greatly affected by its anion, and followed the order [bmim]BF4 < [bmim]CF3SO3 < [bmim]Cl under the same conditions, which is consistent with the ascending order of IL’s hydrogen-bond basicity strengths.
Co-reporter:Yifeng Cao, Qiwei Yang, Huabin Xing, Zongbi Bao, Baogen Su, Yiwen Yang, Qilong Ren
Chinese Journal of Chemical Engineering (October 2014) Volume 22(Issue 10) pp:1141-1144
Publication Date(Web):1 October 2014
DOI:10.1016/j.cjche.2013.05.001
The solubility of nonivamide in dimethyl sulfoxide, methanol, acetone, ethyl acetate, methyl tert-butyl ether, acetonitrile, n-hexane and water over the temperature range of 293.2 K to 323.2 K was measured. The results reveal that the solubility of nonivamide is greatly influenced by the hydrogen-bond basicity of solvent and increases with temperature. The experimental data were correlated with the modified Apelblat equation. The dissolution enthalpy and entropy of nonivamide in different solvents were obtained from the correlation of lnx with 1/T using the van't Hoff equation. The calculated nonivamide solubility is in good agreement with experimental data for most of the solvents.The figure shows the correlation between the solubility of nonivamide (xi) and the hydrogen-bond basicity (β) of the solvent. The molecular structure of nonivamide shows that it contains a benzene ring, a hydrogen-bond acidic phenolic hydroxyl group, a hydrogen-bond basic amide group and a hydrophobic alkyl chain. It is seen that the solubility of nonivamide generally increases as the hydrogen-bonding basicity of the solvent increases, from which it is learned that the hydrogen-bonding interaction between solute and solvent is a key factor that determines the solubility of nonivamide in various solvents.Download full-size image
Co-reporter:Xili Cui, Qiwei Yang, Yijun Xiong, Zongbi Bao, Huabin Xing and Sheng Dai
Chemical Communications 2017 - vol. 53(Issue 36) pp:NaN4918-4918
Publication Date(Web):2017/04/03
DOI:10.1039/C7CC01000A
Here we report a facile and effective strategy for the preparation of ordered mesoporous carbon materials with a high-nitrogen-content (8.1 at%) coating layer through a polymer–ionic liquid assembly strategy. The prepared N-doped mesoporous carbon materials demonstrated enhanced CO2 adsorption capacity (2.29 mmol g−1) compared with non-doped carbon (1.84 mmol g−1).
Co-reporter:Xian Suo, Ling Xia, Qiwei Yang, Zhiguo Zhang, Zongbi Bao, Qilong Ren, Yiwen Yang and Huabin Xing
Journal of Materials Chemistry A 2017 - vol. 5(Issue 27) pp:NaN14123-14123
Publication Date(Web):2017/06/14
DOI:10.1039/C7TA01986F
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; Sβ&γ/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.
Co-reporter:Wenbin Jin, Qiwei Yang, Zhiguo Zhang, Zongbi Bao, Qilong Ren, Yiwen Yang and Huabin Xing
Chemical Communications 2015 - vol. 51(Issue 67) pp:NaN13173-13173
Publication Date(Web):2015/07/01
DOI:10.1039/C5CC03463A
Here we report a novel self-assembly induced solubilization strategy with nanostructured ionic liquids as solvents. Highly ordered mesoscopic structures featuring the solute as a key component, such as liquid crystals, were formed via self-assembly in nanostructured long-chain carboxylate ionic liquids, resulting in extremely high solubilities for sparingly soluble drug molecules.
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