Inorganic Chemistry Frontiers
·
2021
·Vol. 9
·期 1
·165-178
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IF 6.569
Ning Yang,Linjie Lu,Linhua Zhu,Peiwen Wu,Duanjian Tao,Xiaowei Li,Jiahong Gong,Linlin Chen,Yanhong Chao,Wenshuai Zhu
Porous ionic liquids (PILs), with permanent porosity and fluidity, have been drawing great attention in theoretical research and application. Herein, a novel PIL (HPMo@ZIF-8-PIL) was fabricated by dispersing a phosphomolybdic acid-modified zeolitic imidazolate framework-8 (ZIF-8) into an ionic liquid for deep reactive extraction desulfurization. Size calculation results show that 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonylimide) ([Emim][NTf2]) with larger ion sizes cannot occupy pores of ZIF-8. In detail, the structure along with permanent porosity was well characterized by gas absorption and molecule displacement experiments, and it was found that HPMo@ZIF-8-PIL can not only promote the dispersion of the catalytically active sites but also retain the good liquidity and excellent extraction ability of ionic liquids. At room temperature, 100% removal of dibenzothiophene sulfur in a model oil could be achieved within 2 h using HPMo@ZIF-8-PIL and hydrogen peroxide as the catalyst and oxidant, respectively. Besides, the successful preservation of porosity increases the probability of contact between the oxidant and active sites, which is also in favor of the promotion of desulfurization performance. This work offers a new method for the modification of porous frameworks to construct PIL catalysts, which will provide a new insight into the application of PILs.
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NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 14
·11539-11547
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IF 3.201
Jing Gao,Shun Yao,Yu Wang,Zhengbo Hou,Chang Yang,Hang Song
Trichosanthin (TCS) is a kind of basic protein separated from Trichosanthes kirilowii Maxim, which is a good food source for human nutrients and has important uses for health. In this study, a series of imidazole-based ionic liquids (ILs) were chosen as catalysts for TCS hydrolysis in both heating and microwave-assisted modes and the hydrolysis was compared with chlorhydric acid and sulfuric acid together with sodium hydroxide for the degree of hydrolysis (DH) of TCS. It was found that the performance of acidic ILs > neutral ILs > basic ILs; [Hmim][HSO4] among the ILs presented the highest DH which was even better than those of inorganic strong acids. Furthermore, the process of hydrolysis was optimized with 3D-response surface methodology (RSM), and the highest degree of hydrolysis could reach to 48.3% (in heating mode) and 93.9% (in microwave-assisted mode). Finally, D001Na type cation-exchange resins were used in the selective adsorption of amino acid products and ILs in an effluent that could be reused. The hydrolysates from TCS showed an enhanced antioxidant activity which was evaluated in three ways. This study could provide a useful foundation for further research and exploitation of TCS.
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Journal of CO2 Utilization
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2016
·
IF 4.764
Xian-Dong Lang,Yi-Chen Yu,Zheng-Ming Li,Liang-Nian He
Despite recent renaissance of CO 2 chemistry, transformation of CO 2 at ambient conditions remains still of great challenge. In this work, an easily prepared protic ionic liquid e.g. 1,1,3,3-tetramethylguanidinium imidazolide [HTMG][Im] was developed as highly efficient, recyclable and bifunctional catalyst for the carboxylative cyclization of 2-aminobenzonitriles with CO 2 at atmospheric pressure and room temperature. The catalytic protocol was found to be applicable to various 2-aminobenzonitriles bearing electron-withdrawing or electron-donating substituents, affording the corresponding quinazoline-2,4(1H,3H)-diones in moderate to excellent yields. In addition, the catalyst could be conveniently recovered and reused for five cycles with almost consistent activity. Consequently, this process represents an alternative approach for the efficient and greener chemical fixation of CO 2 to afford valuable heterocycles.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Jiuli Han,Lu Bai,Haiyan Jiang,Shaojuan Zeng,Bingbing Yang,Yinge Bai,Xiangping Zhang
Ionic liquids (ILs) have become attractive in membranes for CO2 separation because of the designable structure, high CO2 affinity, and good compatibility and stability. Modification of metal–organic frameworks with ILs is an effective strategy to improve the gas separation performance of mixed matrix membranes (MMMs). In this work, task-specific ionic liquids (TSILs) were incorporated to prepare TSIL@ZIF-67/PIM-1 MMMs and improve CO2 separation performance because of the high CO2 solubility and great compatibility toward ZIF-67 and PIM-1. The TSILs (TMGHIM and TMGHPhO) selectively and reversibly interact with CO2 and improve the interfacial compatibility between ZIF-67 and PIM-1, leading to higher CO2/CH4 and CO2/N2 selectivities than that of the ZIF-67/PIM-1 MMM and the directly blended membrane (TSIL/ZIF-67/PIM-1). The 10 wt % TMGHIM@ZIF-67/PIM-1 MMM shows enhanced CO2/N2 and CO2/CH4 selectivities of 13.7 and 10.5, respectively; meanwhile, the CO2 permeability reaches 12,848.5 Barrer and is 2.5 times that of the pure PIM-1 membrane. The TSIL@ZIF-67/PIM-1 MMMs also show good stability against physical aging.
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SOLID STATE IONICS
·
2018
·
IF 2.751
Dapeng Shang,Jifang Fu,Qi Lu,Liya Chen,Jintao Yin,Xing Dong,Yufeng Xu,Rongrong Jia,Shuai Yuan,Yi Chen,Wei Deng
A series of novel imidazolium-based polyhedral oligomeric silsesquioxane ionic liquids (POSS-ILs) have been successfully synthesized and used to develop new solid polymer electrolytes with high ionic conductivity and wide electrochemical windows. The POSS-ILs are added to the solid polymer electrolytes (SPEs) based on blend of polyethylene oxide (PEO), poly(vinylidene fluoride-hexafluoro propylene) (P(VDF-HFP)), propylene carbonate (PC) and lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) to alter the morphology, ionic conductivity , electrochemical windows properties. The results from scanning electron microscope (SEM), energy-dispersive x-ray spectrometry (EDXS) mapping and X-ray diffraction (XRD) indicate that POSS-ILs are uniformly distributed in the SPEs and form amorphous area by significantly inhibiting the crystallization of host polymer. The electrochemical studies indicate that the addition of POSS-ILs increases the ionic conductivity up to 3.9 × 10 −4 S cm −1 at 22 °C and 1.5 × 10 −3 S cm −1 at 62 °C. The electrochemical windows of POSS-ILs based SPEs are stable up to 5.0 V. As a result, the lithium-ion battery cell prepared using the POSS-ILs-SPE showed a good cycle performance and reversible capacity recovery behavior. These indicate POSS-ILs based SPEs would be good candidate to replace the conventional organic liquid electrolytes for lithium ion batteries.
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JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Jiangnan Wang,Long Li,Jinli Zhang,Xueqin Li
The construction on the interconnected network can be considered as a potential strategy for boosting CO 2 transport in mixed matrix membranes (MMMs). In this study, poly (ionic liquids)/ZIF-8 (PIL/ZIF-8) was synthesized and incorporated into sulfonated poly (ether ether ketone) (SPEEK) matrix to fabricate MMMs for rapid CO 2 transport. Wherein, ZIF-8 with a highly porous framework within PIL/ZIF-8 can efficiently capture CO 2 and allow CO 2 simultaneously transport in multi routes, thus improving CO 2 separation performance of SPEEK/PIL/ZIF-8 MMMs. PIL in PIL/ZIF-8 can guide the rapid transport of CO 2 in an orderly manner with the help of the anion CO 2 carriers (Cl − ) on the PIL chains, accelerating CO 2 transport in the MMMs. And the interconnected network was constructed by incorporating PIL/ZIF-8 in MMMs, which was endowed with the excellent CO 2 separation performance. And the CO 2 permeability and CO 2 /CH 4 selectivity of SPEEK/PIL/ZIF-8-7 MMM were 1641 ± 41 Barrer and 32 ± 0.9, respectively, approaching the 2019 upper bound. It implied that the construction on the interconnected network in MMMs had great potential for rapid CO 2 transport.
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产品关联
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高影响因子
RSC Advances
·
2022
·Vol. 12
·期 6
·3416-3422
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IF 4.036
Jing Yuan,Ningning Zhou,Jieyu Wu,Tianxiang Yin,Yunbin Jia
Ionic liquids, especially the cholinium-amino acid-based ionic liquids (CHAAILs), have recently been found to be effective ingredients in formulation of transdermal drug delivery system. In this work, we synthesized six CHAAILs, and investigated their ability to enhance the solubility and permeation of two active pharmaceutic ingredients (APIs), i.e. ferulic acid and puerarin. The solubility measurements showed that a low amount of CHAAILs can significantly increase the solubility of APIs. Moreover, the effective enhancement of permeation of APIs across a polyethersulfone (PES) membrane was achieved at low concentration (4 mg ml−1) of CHAAILs. It is more worthwhile that the presence of CHAAIL brings much less cytotoxicity as compared to traditional types of ionic liquids. Therefore, CHAAILs can be considered as great potential candidates of green and effective additives in transdermal drug delivery systems.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Shaojuan Zeng,Junli Wang,Pengfei Li,Haifeng Dong,Hui Wang,Xiaochun Zhang,Xiangping Zhang
The emerging of ionic liquids (ILs) provides a promising way to efficiently separate ammonia (NH 3 ) and simultaneously recover NH 3 due to their negligible volatility, good affinity with NH 3 and designable structures. However, the relatively high viscosities of ILs and the limited gas-liquid interface severely affect gas diffusion in ILs, which hinders their practical use in industries. In this work, in order to overcome the mass-transfer limitations of ILs in gas separation, three metal ILs (MILs), [Bmim] 2 [CuCl 4 ], [Bmim] 2 [NiCl 4 ] and [Bmim] 2 [Co(NCS) 4 ], with good affinity toward NH 3 were incorporated into porous silica gels with large surface area and abundant hydroxyl groups, by an impregnation-vaporization method to form novel MIL@silica gel composites for rapid, efficient and reversible adsorption of NH 3 . The FT-IR and BET results indicated that the prepared adsorbents with different loadings of MILs are mesoporous composites. The [Bmim] 2 [Co(NCS) 4 ]@silica gel composites not only show much higher NH 3 capacity and NH 3 selectivity than pristine silica gel and faster adsorption rate than the corresponding pure MILs, but also exhibit excellent reversibility. The highest capacity of NH 3 adsorption up to 99.808 mg NH 3 ·(g adsorbent) −1 in 15 min was obtained when the loading of [Bmim] 2 [Co(NCS) 4 ] in the MIL@silica gel composite was 48.89 wt%, which could be attributed to the synergistic interaction of the complexation and hydrogen bonding between cobalt coordinated anion and NH 3 as well as mesoporous structures. Moreover, the NH 3 absorbed by the [Bmim] 2 [Co(SCN) 4 ]@silica gel can be completely released in 15 min, and no obvious losses in NH 3 capacity were detected during five adsorption and regeneration cycles, indicating great potentials as adsorbents for NH 3 separation applications.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yu Wang,Yunlei Shi,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Xiaopeng Xuan,Jianji Wang
Ammonia (NH3) is a promising clean energy because of its high hydrogen density and carbon-free nature. Therefore, the capture, storage, and desorption of NH3 have received widespread attention in recent years. However, achieving highly efficient capture and release of NH3 remains a challenge. Herein, an efficient strategy is proposed to fabricate defects in a metal–organic framework (UiO-66) by using ionic liquid as a modulator for the first time. It is found that the NH3 adsorption capacity of the optimal defective UiO-66 is up to 1.60 times that of the pristine UiO-66 because of 16.8% of the linker missing. It is noteworthy that the adsorption of NH3 in the defective UiO-66 is completely reversible under conventional pressure-swing conditions, and more than 95% of the NH3 uptake capacity can be maintained after 30 adsorption–desorption cycles. It is revealed that the enhanced coordinating interaction of NH3 to Zr4+ and hydrogen bonding interactions between NH3 and oxygen-containing groups in the framework are the main driving forces for the substantially increased NH3 uptake. In addition, the strategy developed here is green and simple for manufacturing defects, which opens up a new pathway to the preparation of a wide range of solid adsorbents and catalysts.
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ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Yin Qiu,Liming Wang
Ionic liquids (ILs) with promising application are likely to become ubiquitous contaminants in water environment for their high hydrophilicity, low biodegradability , and especially its potential toxicity. In this work, we have investigated photochemical transformation of six imidazolium ILs for fate prediction and ecological risk assessment . We found that the reaction rates of the ILs with •OH, CO 3 •─ and 1 O 2 enhanced with their increasing alkyl chain and varied slightly with the paired anions. Meanwhile, modelled results under different scenarios indicate that the primary contributors to transformation of the ILs are triplet-stated dissolved matter ( 3 CDOM*), •OH and CO 3 •– . Besides, the overall half-lives of the ILs can reach 670 days, which indicates persistence of these ILs in the environment. Products for ILs in reaction with •OH and triplet-stated sodium anthraquinone-2-sulfonate ( 3 AQ2S*) were probed by UHPLC-Q-TOF-MS/MS and there is a difference between their products: Products by •OH are likely formed by hydrogen abstraction from the side alkyl chain, followed by dehydrogenation , hydroxylation and carbonylation, while one of the products by 3 AQ2S* is formed by dihydroxyl-addition of the imidazolium ring. Furthermore, the ILs and its products were estimated to have toxicity and non-readily biodegradability, suggesting potential eco-risk for the environmental water.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Shenyao Wang,Xiaoyu Lv,Zhenyu Zhao,Yixin Chen,Zhong Chen,Wenjun Lin,Haoran Li,Congmin Wang
A novel method of using anion-functionalized ionic liquids (ILs) with high NO absorption capacity and reversibility for the capture and in situ oxidation of low-concentration NO was established. For the mixed gas containing 0.25% NO, the accumulation rate of nitric acid in these ILs was significantly higher than that in the conventional ILs; after absorption and oxidation reached equilibrium, the molar ratio of HNO3 to [P4446][PhSO3] was 0.86, which was 5 times as high as that of the conventional IL. Therefore, the problems of low efficiency and poor reversibility of traditional ILs in the absorption and oxidation process were solved. Through absorption and oxidation experiments, quantum chemical calculation, NMR, and time-resolved in situ ATR-FTIR spectroscopic investigation, the results demonstrated that such a high accumulation rate of HNO3 originated from high uptake of NO through multiple-site interaction. Moreover, high reversibility is attributed to low volatility of conjugated acid of anions and decreased basicity of O sites on anions. We believe that such highly efficient and reversible conversion of low-concentration NO to HNO3 by ILs provides a new strategy for improving atomic economy of fossil fuel combustion, that is, converting post-combustion pollutants to good valuable chemicals.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Litian Wang,Jie Chen,Shuai Wang,Tongyao Zhou,Dan Li,Cuiping Li,Lirong Qian,Yang Xiong,Lin Miao,Zhiyong Xie
Protic ionic liquids (PILs) have emerged as innovative solvents with significant potential for CO 2 capture and transformation, presenting a sustainable alternative to conventional methods which often involve energy-intensive processes or environmentally detrimental chemicals. Herein, a novel strategy for CO 2 capture and conversion at mild conditions using non-stoichiometric protic ionic liquids (NPILs) was demonstrated for the first time. These NPILs, employed as sorbents, solvents, and catalysts, were composed of imidazole (Im) and 1,8-diazabicyclo [5.4.0] undec-7-ene (DBU) in various ratios. Correlations between the mole ratio of DBU/Im and physicochemical properties such as viscosity, conductivity, thermal stability, and the distribution of neutral and ionic species were systematically investigated. Effects of the absorption temperature and CO 2 partial pressure on the absorption capacity were also studied. Different absorption mechanisms, including carbonate and carbamate pathways, were analyzed using FT-IR and NMR spectroscopy. Moreover, the fixed CO 2 could be catalytically converted to quinazoline-2,4(1H,3H)-diones under exceptionally mild reaction conditions (1 atm, 50 °C, metal-free process). A plausible reaction mechanism involving simultaneous CO 2 activation and substrate activation for the transformation of CO 2 into quinazoline-2,4(1H,3H)-diones was verified through NMR spectra. It is believed that the new insights into the CO 2 mechanism will facilitate the rational design of functional ionic liquids for CO 2 capture, utilization, and storage in the future.
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