JOURNAL OF CHROMATOGRAPHY A
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2019
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IF 3.858
Fengli Chen,Yao Xiao,Bingwen Zhang,Ruigang Chang,Duqiang Luo,Lei Yang,Yongfan Yang,Dongmei Liu
In this work, synthesized magnetic silicone loaded with ionic liquid (Fe 3 O 4 @SiO 2 @IL) particles combined with gas-liquid-solid magnetically stabilized bed (GLS-MSB) were applied to enrich flavonoids from tree peony petal extraction solution. The magnetic core (Fe 3 O 4 ) encased in silica was conducive to its rapid and efficient separation, and the modification of silica with ionic liquids (ILs) could provide the functional groups for selective adsorption of flavonoids. Furthermore, the magnetic materials were evenly dispersed in the GLS-MSB system, realizing the adequate contact and causing the positive influence on the result. After physicochemical characterization, the prepared Fe 3 O 4 @SiO 2 @IL (IL=VBimBr) particles were validated in the enrichment performance of flavonoids, including the type of ionic liquid loaded, desorption solution, adsorption and desorption kinetics. The adsorption kinetics obeyed the pseudo-second-order model, the adsorption isotherms were consistent with the Langmuir equation, and the adsorption process was spontaneous and exothermic. Additionally, the dynamic processes using GLS-MSB packed with Fe 3 O 4 @SiO 2 @IL particles were evaluated systematically, deriving the optimum conditions (5 mL/min liquid flow rate, 130 mL Loading amount and 42.55 Oe magnetic field intensity) and improving the purity of flavonoids. After enrichment, the Fe 3 O 4 @SiO 2 @IL particles were successfully recycled and reused. Overall, the developed method offers a great potential for the enrichment of flavonoids from natural materials.
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JOURNAL OF MEMBRANE SCIENCE
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2026
·
IF 8.8
Chao Tang,Guowei Yang,Bing Wu,Guangjian Chai,Dian Qu,Chun Chen,Zhihong Yang,Jian Sun,Jianmei Xu,Zhiquan Chen,Qihang Wang,Wei Zhou
PIL modification tailors MOF-808 pore environment and CO 2 -affinitive sites. • PIL-modified MOF-808 improves filler-Pebax interfacial compatibility. • PALS reveals reduced FFV in PIL-modified MOF-808/Pebax MMMs. • The optimized MMM surpasses the 2008 CO 2 /N 2 Robeson upper bound. • CO 2 solubility gain outweighs diffusivity loss despite reduced free volume. Carbon capture is an important strategy for mitigating climate change, and membrane-based CO 2 separation offers advantages such as low energy consumption, operational simplicity, and continuous operation. Incorporating metal-organic frameworks (MOF), improving the interface between MOF and polymers, and introducing sites with CO 2 affinity are effective approaches for enhancing mixed matrix membranes (MMMs) performance. In this study, poly(ionic liquid) (PIL)-modified MOF-808 fillers were synthesized through in situ polymerization and incorporated into Pebax membranes. The PIL modification adjusted the pore environment of MOF-808, introduced imidazolium and -COOH groups, and strengthened interactions between the filler and Pebax, thereby restricting Pebax chain mobility. The optimized MMM exhibited a CO 2 permeability of 124.57 Barrer at 0.1 MPa and 35 °C, with CO 2 /N 2 selectivity surpassing the 2008 Robeson upper bound and CO 2 /CH 4 selectivity also substantially improved. Positron annihilation lifetime spectroscopy (PALS) revealed a reduction in fractional free volume compared with pristine Pebax, while time-lag analysis showed a corresponding decrease in gas diffusivity. In contrast, the CO 2 solubility coefficient increased markedly because of the CO 2 affinity introduced by PIL. The increase in CO 2 solubility was larger than the loss in diffusivity, leading to enhanced CO 2 permeability and selectivity despite reduced free volume. By combining PALS with time-lag analysis, nanoscale free volume evolution was connected with diffusion and solubility contributions. These results show that PIL-modified MOF-808 changes the balance between diffusivity and solubility in MOF/Pebax MMMs and clarify why CO 2 transport can be improved even when free volume and diffusivity decrease. Download: Download high-res image (432KB) Download: Download full-size image
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Liling Wang,Yanbin Wang,Yuchuan Qin,Yifeng Zhou
Waters contaminated with pesticides poses a potential hazard to ecosystems and human health, so sensitive and efficient analytical methods are essential for water monitoring. Herein, in order to efficiently extract six commonly used herbicides, a novel ionic liquid covalent organic framework (IL@COF) was prepared using a simple room-temperature synthesis in this study. As an adsorbent for solid phase extraction (SPE), the mesoporous material exhibits rapid adsorption performance for six typical herbicides from water samples. Under the optimal experimental conditions, wide linearities (500 ∼ 20,000 μg L –1 ) and low limits of detection (prometryn: 17.9 μg L –1 ; metribuzin: 36.7 μg L –1 ; bentazon: 14.5 μg L –1 ; isoproturon: 18.0 μg L –1 ; acetochlor: 19.6 μg L –1 ; butachlor: 37.1 μg L –1 ) for six analytes were obtained via high performance liquid chromatography (HPLC). The adsorbent has stable physical and chemical properties and can be reused for 10 times after effective elution. The applicability of this method is further evaluated by analyzing ten kinds of real water sample. The recoveries of six kinds of herbicides ranged from 85.3 % to 122.9 %. The mechanism of adsorption is the interaction between hydrogen bond acceptor and donor. These results indicate that HPLC after SPE with a new type of IL@COF as the SPE adsorbent is a promising technique for the simultaneous detection of six pesticides in environmental water samples.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lang Wu,Hong Qin,Songhua Zhou,Ziming Luo,Yang Xiao,Huan You,Qian Lin,Hongyan Pan,Keliang Wang
Direct synthesis of hydrogen peroxide (H 2 O 2 ) from hydrogen (H 2 ) and oxygen (O 2) is an ideal industrial method to replace the anthraquinone oxidation process for H 2 O 2 production, however, it is still limited by low H 2 O 2 selectivity and productivity. The electronic structure and wettability of the catalyst are crucial factors that affects the catalytic performance. This study demonstrates that binding hydrophobic 1-butyl-3-methylimidazolium-hexafluorophosphate ([Bmim]PF 6 ) ionic liquid on the surface of Pd nanoparticles (Pd NPs) can increase the content of electron-deficient state Pd (Pd 2+ ) at the active site, which exhibits excellent catalytic performance (90.8% H 2 O 2 selectivity and 8828.6 mmol g Pd −1 h −1 H 2 O 2 productivity). The results of XPS, O 2 -TPD and DFT show that the increase of Pd 2+ content effectively inhibits the O-O bond dissociation of O 2 *, OOH*, and HOOH*, thus improving H 2 O 2 selectivity and productivity. Moreover, the hydrophobicity of [Bmim]PF 6 induces a change in the three-dimensional hydrophilic microenvironment of the Pd active site, reducing the energy required for HOOH* desorption from the active site by 0.07 eV (from 0.53 eV to 0.46 eV). This is useful in preventing further hydrogenation and decomposition of HOOH*. TEM characterization suggests that the steric hindrance of [Bmim]PF 6 impedes the aggregation of Pd NPs during the reaction, resulting in different cyclic stability of Pd/OCNT and Pd [Bmim]PF 6 /OCNT.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xuemei Li,Yang Shen,Fangyu Jin,Jingbo Zhang,Yanyan Yang,Xiaoshu Qu
Nuclear waste management and nuclear energy generation require the proper disposal of 129 I and 131 I, which are radioactive isotopes of iodine. For recognition of different types’ iodine, a magnetic poly (ionic liquid)s (Fe 3 O 4 @SiO 2 -MPS-PILs) was formed by the selected imidazole ionic liquid monomer and core–shell Fe 3 O 4 @SiO 2 -MPS via free radical polymerization. The resulting adsorbent containing plenty of imidazole N-heterocycle units, benzene rings, and ionic bonds in the backbones was suitable for simultaneously adsorbing iodine molecules and iodide ions. The adsorption mechanisms for iodine in cyclohexane and iodide ions from aqueous solution were based on charge transfer and ion exchange mechanisms, respectively. The adsorption equilibrium for iodine in cyclohexane was attained at 12 h, and the kinetics of iodine adsorption closely followed the pseudo-second-order model. Iodine adsorption on Fe 3 O 4 @SiO 2 -MPS-PILs was best described by Langmuir model with a maximum iodine adsorption capacity of approximately 714.29 mg g −1 . Iodide ions adsorption was best explained with Freundlich model and a maximum adsorption capacity of 335.80 mg g −1 was achieved in an iodide solution with a 500 mg L –1 concentration. Notably, Fe 3 O 4 @SiO 2 -MPS-PILs retained over 90 % of its original adsorption performance after the 5th cycle. This work proves that the adsorbent Fe 3 O 4 @SiO 2 -MPS-PILs was efficient and recyclable, and has good application prospects in the practical treatment of iodine and iodide.
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Reaction Chemistry & Engineering
·
2023
·Vol. 8
·期 12
·3124-3132
·
IF 3.9
Chenhua Shu,Min Zhao,Hua Cheng,Yajie Deng,Pierre Stiernet,Niklas Hedin,Jiayin Yuan
A type-III porous liquid based on zeolitic imidazolate framework-8 (ZIF-8) and an ionic liquid trihexyltetradecylphosphonium bis(trifluoromethylsulfonyl)imide ([THTDP][BTI]) was synthesized and used for the desulfurization of model diesel. The desulfurization effect by ZIF-8/[THTDP][BTI] combined both the adsorptive desulfurization by ZIF-8 and the extraction desulfurization by [THTDP][BTI]. The removal of the three chosen aromatic organic sulfides by the ZIF-8/[THTDP][BTI] porous liquid followed the order of dibenzothiophene (73.1%) > benzothiophene (70.0%) > thiophene (61.5%). It was further found that deep desulfurization could be realized by ZIF-8/[THTDP][BTI] through triple desulfurization cycles and ZIF-8/[THTDP][BTI] can be regenerated readily. The desulfurization mechanism was explored further in detail by conformation search and density functional theory calculations. Calculations supported that the large molecular volume of [THTDP][BTI] excluded itself from the cavities of ZIF-8, making the pores of ZIF-8 in the porous liquid unoccupied and accessible by other guest species, here the studied organic sulfides. These calculations indicate that the van der Waals interactions were the main interactions between ZIF-8/[THTDP][BTI] and specifically benzothiophene. This work supports that the porous liquid ZIF-8/[THTDP][BTI] could potentially be used for desulfurization of diesel in industry.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
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IF 8.2
Yan Li,Ying Dai,Wei Dai,Feiqiang He,Zhuyao Li,Xing Zhong,Qinqin Tao
Uranium and thorium of symbiotic relationship commonly appear in one kind of raw or spent ore. The simultaneous enrichment toward both metals in the first step is essential during many hydrometallurgy processing. Therefore bifunctional solid-state ionic liquid supported amidoxime chitosan (ACS) adsorbents were developed to simultaneously adsorb the two metal from the aqueous solution. The adsorption capacity of the bifunctional adsorbents toward uranium and thorium were significantly superior to the ionic liquid-free amidoxime chitosan, obviously proving the synergistic effect. For both uranium and thorium, the adsorption capacity in the consequence of ACS-[N 4444 ][DEHP], ACS-[N 4444 ][EHEHP], ACS-[N 1888 ][DEHP] and ACS-[N 1888 ][EHEHP] prove the steric effect and P O bonding played important roles in the adsorption. Study on isotherms and kinetics demonstrated the adsorption of ionic liquid-ACS adopted monolayer and chemical way. The Δ G o of very small negative values highlighted ionic liquid-ACS were prone to adsorb uranium and thorium. The study showed feasibility of bifunctional solid-state ionic liquid supported amidoxime chitosan adsorbents for Th(IV) and U(VI).
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 19
·7743-7755
·
IF 9.8
Bihua Chen,Shiguo Zhang,Yan Zhang
Developing a simple and efficient heterogeneous catalyst for the cycloaddition of epoxides with CO2 under atmospheric pressure and cocatalyst-/metal-/solvent-free conditions remains a great challenge. Herein, poly(ionic liquid)s (P-[VRIm]Br-crosslinker-x) with unique adsorption-swelling ability toward epoxides are designed and facilely synthesized via free radical polymerization in water. The adsorption-swelling of epoxides by P-[VRIm]Br-crosslinker-x is controllable, reversible, and widespread, resulting from the strong interactions between the poly(ionic liquid)s and epoxide molecules, especially the hydrogen-bonding interaction. Superior CO2 cycloaddition is realized in the P-[VRIm]Br-crosslinker-x catalyst through the adsorption-swelling effect. Specifically, P-[VC6Im]Br-C8-5% with 54.1 mmol g−1 adsorption-swelling ability toward styrene oxide achieves 89.3% yield and >99% selectivity in the cycloaddition of styrene oxide with CO2 to styrene carbonate under mild conditions (1 atm, 80 °C) without cocatalyst/metal/solvent consumption. Moreover, P-[VC6Im]Br-C8-5% can be easily recovered by deswelling, and shows good reusability and stability after five cycles for a total of 180 h. The adsorption-swelling property of P-[VRIm]Br-crosslinker-x to epoxides not only prompts the active centers to be fully exposed to the reactants but also induces the enrichment of epoxides during the whole catalytic process, thus accelerating the CO2 cycloaddition reaction rate. This work furnishes new insights for improving the activity of CO2 cycloaddition and would guide the design of efficient poly(ionic liquid) catalysts for atmospheric CO2 conversion.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Ximan Bu,Linlin Wu,Xiaofeng Ma,Wenjing Diao,Duyou Lu
It remains challenging to develop hydrogel electrolyte with integrated superior mechanical properties and ionic conductivity for high performance flexible supercapacitors. Herein, copolymer hydrogels are prepared via a one-step polymerization of acrylamide (AM), 3-(1-vinyl-3-imidazolio) propanesulfonate (VIPS) zwitterionic monomer and 3-sulfopropyl methacrylate potassium salt anionic monomer (SPMA). On one hand, the ionic interaction as reversible “sacrificial bonds” provided by VIPS and SPMA through SO 3 −—H 3 N+ makes these hydrogels tough (fracture energy 3.8 MJ m −3 ), stretchable (fracture strain 5100%), flexible and self-recoverable (~98% recovery efficiency after 1000% strain deformed). On the other hand, high ionic conductivity (3.1 S m −1 ) is achieved due to the efficient ion migration channels derived from the zwitterionic copolymer with high hydration capacity. Based on this hydrogel, the as-prepared flexible supercapacitor not only exhibits high discharge capacitance of 108.8 F g -1 at 1 A g -1 , and retains ~99% of its capacitance after 1000 cycles, but also achieves encouraging performance at subzero temperature due to the prevention of ice formation by zwitterionic polymer. This hydrogel can be easily functionalized with ionic liquid or other functional materials to extend their practical application.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Fan Xu,Haolin Li,Bingyu Tian,Kun Cui,Rui Dong,Mingjin Fan,Meirong Cai,Feng Zhou,Weimin Liu
Owing to the green, high-performance, and application-specific work conditions, water-based lubricating systems show unlimited potential for chemical engineering development. The interfacial behavior of functional additives in aqueous systems is complex and variable due to polarity and interfacial activity, thus showing important research significance. Herein, five novel ionic liquids were synthesized; their unique interfacial behavior in the polar water system contributes a lot to the advanced corrosion resistance and the improved extreme pressure-bearing capacity. The polar groups in the molecular structure of ionic liquids can adsorb preferentially in competition with water molecules, resulting in the formation of an adsorption layer with a high elastic modulus on the metal surface. Benefiting from the tribochemical reaction and the strong polar adsorption effect, the tribofilm at the sliding asperity exhibited effective antiscuffing and antiwear performance. Moreover, their characteristic cationic groups enrich the driving force of the molecular self-assembly process and enhance the ability to form ordered molecular aggregates, whose behavior in an aqueous system facilitates super-robust lubricity. This work can promote the in-depth understanding, future design, and optimization of the aqueous lubricating system, providing content enrichment and expansion for the lubrication technology for harsh service conditions.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 6
·1869-1881
·
IF 1.6
Zhang Na,Yang Miao,Zhang Manman,Du Jifu,Bao Qiburi,Zhao Long,Dong Zhen
Amphiphilic double poly(imidazole ionic liquid) grafted silica (SMIL-n) was prepared by radiation grafting of hydrophilic 1-vinyl-3-ethylimidazolium bromide and hydrophobic 1-vinyl-3-octylimidazolium bromide at different ratio onto silica. The adsorption behavior of SMIL-n was investigated. The adsorption equilibrium could reach less than 45 min, and their adsorption capacity were 152–171 mg/g obtained from Langmuir model. The selectivity of SMIL-n to ReO 4 − increased with the increasing content of hydrophobic ionic liquid. SMIL-n displayed good reusability, excellent acid resistance and irradiation resistance. Particularly, SMIL-n showed promising for ReO 4 − uptake from simulated contaminated Beishan groundwater and radioactive wastewater.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 18
·e53802
·
IF 3
Xiaoyu Meng,Qiwang Peng,Jihong Wen,Kai Song,Luman Peng,Tianyu Wu,Chuanbo Cong,Haimu Ye,Qiong Zhou
In vanadium redox flow battery (VRFB). Sulfonated poly(ether ether ketone) (SPEEK) is viewed as a promising alternative to Nafion as a material for vanadium liquid flow battery membrane, due to its low cost and high proton conductivity. However, SPEEK membranes have a Trade-Off effect of proton conduction and ion selectivity, which limits the performance of VRFB. Here, we exploited the Donnan effect of imidazole cations in ionic liquids (ILs) to improve the ion selectivity of SPEEK membrane. In addition, used porous covalent organic framework materials (COF) with sulfonic acid functional groups to immobilize ionic liquids, which reduced the loss of ILs. The ion selectivity of the SPEEK membrane was further improved. As a result, the cell performance of the composite membrane is improved. At a constant current density of 40 mA cm −2 , SPEEK/IL-5@TpPa-SO 3 H-3 membrane exhibits high coulombic efficiencies (CE: 98.43%) and energy efficiencies (EE: 91.7%). Furthermore, the energy efficiency of the SPEEK/IL-5@TpPa-SO 3 H-3 membrane decreases only 2.1% after 60 charge/discharge cycles at 100 mA cm −2 . Our work proposed a cost-effective, high-performance membrane for VRFB.
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