JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xinmeng Zhuang,Xinfu Chen,Lin Xu,Shuainan Liu,Yanjie Wu,Zhichong Shi,Qingqing Zhou,Bo Li,Haixia Yan,Peter Reiss,Hongwei Song
Long-term stability remains a great challenge for metal halide perovskite solar cells (PSCs). The utilization of ionic liquids (ILs) is a promising strategy to solve the stability problem. However, few studies have focused on controlling the halide anions of ILs, in which different organic cations can modulate the melting point of ILs and film crystal growth. Here, ILs with a 1-ethyl-3-methylimidazolium (EMIM + ) cation and different halide anions (X = Cl, Br, and I) are employed in inverted PSCs. The results show that EMIMX can form a 1D passivation layer by the in situ growth technique and influence the surface morphology of the perovskite film. These EMIMX-treated layers simultaneously suppress the surface defects and nonradiative energy losses and improve the hydrophobic properties. As a result, a power conversion efficiency (PCE) of 20.0% is obtained for the EMIMBr-modified PSCs compared to 18.06% for the control device. Moreover, the unencapsulated devices maintain more than 90% of their initial PCE over 3000 h under ambient air, which is among the best long-term stabilities reported for NiO x -based inverted PSCs. It also retains 74.2% and 49.5% of the initial PCE value after aging under harsher conditions, such as an 85 ± 5% relative humidity (RH) environment and at 85 °C for 48 h, respectively.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Jiuli Han,Haiyan Jiang,Shaojuan Zeng,Yinge Bai,Xiangping Zhang,Lu Bai
Mixed matrix membranes (MMMs) have drawn much interest in CO 2 separation due to their excellent separation performance, mechanical property, and desirable processability. However, obtaining highly compatible MMMs is a great challenge and is vital to avoid the loss of the separation selectivity of the MMMs. In this work, superbase ionic liquid (1,8-diazabicyclo[5,4,0]undec-7-ene imidazole ([HDBU][Im])) was used as a wetting agent to increase the interfacial compatibility between ZIF-67 and PIM-1, hence improving the membrane gas separation. [HDBU][Im] embeding into the MMMs could efficiently enhance the compatibility and diminish the interfacial voids. Furthermore, incorporating 5 wt% [HDBU][Im]@ZIF-67 nanocomposite into the PIM-1 matrix improves the gas permeability and CO 2 selectivity. The separation performances under the different temperatures were also conducted and showed that reducing temperature slightly decreases the gas permeability but significantly increases the CO 2 /CH 4 selectivity via enhancing the CO 2 solubility. The permeation active energies, diffusivities and solubilities were obtained to explain the gas permeate mechanism.
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Biomass Conversion and Biorefinery
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2022
·Vol. 13
·期 13
·11947-11957
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IF 4.05
Xing Xiu,Zhou Zi-Wen,Wei Yun-Jie,Liu Yan-Hong,Li Kun,Yu Xiao-Qi,Wang Na
The process of jatropha oil transesterification was studied for biodiesel production. Rhizomucor miehei lipase (RML) immobilized on 3-aminopropyltriethoxysilane functionalized magnetic Fe 3 O 4 was employed as a biocatalyst. The immobilized lipase was confirmed by scanning electron microcopy (SEM), Fourier transform infrared spectra (FT-IR), thermogravimetric analysis (TGA), vibrating sample magnetometer (VSM), and confocal laser scanning microscopy (CLSM) techniques. The efficient biodiesel synthesis in ionic liquids using immobilized RML was demonstrated. Fifteen kinds of ionic liquids based on different alkyl chain lengths of the methyl imidazolium cation ([C 2 MIM], [C 4 MIM], [C 8 MIM], [C 12 MIM], and [C 16 MIM]) combined with [NTf 2 ], [N(CN) 2 ], [PF 6 ] or [BF 4 ] anions were assayed as reaction media for RML producing biodiesel. The highest synthetic activity of immobilized RML appeared in [BMIM][PF 6 ], which is more than five times higher than the free enzyme. The enzyme catalytic activity remained 60% even after the magnetic nano-biocatalyst and ionic liquid had been reused 5 times in a 48-h reaction cycle. In addition, the immobilized enzyme exhibited excellent storage stability with almost no decrease in catalytic activity after storing at − 20 °C for 98 days.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Han Jia,Shaoyan Wang,Yingbiao Xu,Tingyi Wang,Lingyu Zhang,Jinyong Song,Xuehao Zhang,Lin Song,Haidong Jia,Hui Yan
Ionic liquids are regarded as the promising and efficient additives to use in various aspects of petroleum industry , especially in chemical EOR. In this investigation, three novel fatty acid ionic liquids (FAILs), methyltrioctylammonium octanoate ([N 8881 ][C 8:0 ]), methyltrioctylammonium laurate ([N 8881 ][C 12:0 ]) and methyltrioctylammonium palmitate ([N 8881 ][C 16:0 ]), were selected and evaluated for their performances in terms of surface/interfacial activity, temperature and salt resistances. The three FAILs could cause remarkable reduction of surface tension to ~30mN/m in their aqueous solutions, and the [N 8881 ][C 8:0 ] with the shortest anionic alkane chain exhibited the greatest surface activity among three FAILs. Then the size-match effect and intermolecular interaction were employed to explain the abnormal variations, which were confirmed by the control experiments using mixed surfactants and the molecular dynamics simulation . It was found that the binding energy in [N 8881 ][C 8:0 ] (−28.961 kcal/mol) was larger than that in [N 8881 ][C 16:0 ] (−22.942 kcal/mol), which should be responsible for their different surface activity. Moreover, the crude oil/water interfacial tension (IFT) could be decreased to the much level (4.9 ×10 −3 mN/m and 1.7 × 10 −2 mN/m) even at high-temperature conditions (80 °C) and at high-salinity conditions (100,000 mg/L), indicating the FAILs might be the ideal candidate for the EOR used surfactants with great temperature and salt tolerances. Meanwhile, the variations of IFT results further verified our proposed mechanism.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Qingqing Zhang,Miao Ren,Yunqing Liu,Chaoyue Zhang,Yihang Guo,Daiyu Song
A series of Brønsted acidic ionic liquids (BAILs) functionalized hollow organosilica nanospheres ([C 3/4 Im][OTs/OTf]-Si( Et )Si, C 3/4 = Pr / Bu SO 3 H) were synthesized by two steps. The process involved the preparation of hollow nanosphere supports via a toluene-swollen sol-gel co-condensation of 1,2-bis(trimethoxysilyl)ethane and 3-chloropropyltriethoxysilane in the presence of F127, and followed by a successive quaternary ammonization and protonation with imidazole , 1,3-propane/1,4-butane sultone and trifluoromethane sulfonic acid/ p -toluenesulfonic acid. The adjustable acid property, hollow inner diameter (5–15 nm) and shell thickness (5–9 nm) of [C 3/4 Im][OTs/OTf]-Si( Et )Si are achieved by introducing different organic acids and controlling toluene concentration, respectively. The [C 3/4 Im][OTs/OTf]-Si( Et )Si were applied in selective conversion of fructose to 5-hydroxymethylfurfural (HMF) and 5-ethoxymethylfurfural (EMF) under microwave heating. Under the optimized conditions, the [C 4 Im][OTs]-Si( Et )Si 3.0 nanospheres with the largest inner diameter and the smallest shell thickness exhibit the highest HMF yield (79.4%, 15 min) in fructose dehydration. And the [C 3 Im][OTf]-Si( Et )Si 0.5 nanospheres with the highest acid strength possess the highest EMF yield (70.4%, 30 min) in fructose ethanolysis. The high Brønsted acid-site density and acid strength of [C 3/4 Im][OTs/OTf]-Si( Et )Si catalysts accompanied by high microwave heating energy lead to excellent dehydration/ethanolysis activity. The product selectivity strongly depended on the BAILs structures and morphological characteristics of the catalyst. More importantly, the [C 3/4 Im][OTs/OTf]-Si( Et )Si can be reused three times without changes in leaching of BAILs, due to strong covalent bond between BAILs and silicon/carbon framework. This work will provide a simple strategy of chemically bonded BAILs on suitable supports as efficient solid acids, and an approach of combining morphology-controlled solid acids with microwave-heating for catalytic conversion of biomass/derivatives to fuels and value-added chemicals.
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APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Jiangtao Peng,Haowei Sun,Jian Wang,Peiping Zhang,Weikun Ning,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Shiding Miao
A type of clay-supported catalysts were developed for conversion of CO 2 by encapsulating ZnBr 2 -based Lewis acidic ionic liquids (ZnBr 2 /IL) in halloysite (Hal) via a one-step strategy. The Lewis acidic ionic liquid was loaded within enlarged lumens of Hal via acid treatment, and the mesoporous structure was found to benefit for CO 2 storage/conversion. The composite ZnBr 2 /IL@P-Hal was found to have an adsorption capacity (6.43 cm 3 /g) of CO 2 via adsorption/desorption isotherm measurements. The composite ZnBr 2 /IL@P-Hal showed excellent catalytic performance (TOF value was 1747.7 h −1 ) for coupling of CO 2 with epoxides to produce propylene carbonate under the lack of any cocatalyst . Kinetic investigations indicated the reaction followed an order of one, with respect to catalyst ZnBr 2 /IL@P-Hal. The overall pathway of CO 2 cycloaddition was theoretically validated via DFT calculations. These experimental and computational efforts deepen comprehension of the rational design of clay-based catalysts for CO 2 cycloaddition, further elucidated halloysite was a promising support.
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ChemistrySelect
·
2023
·Vol. 8
·期 45
·e202304285
·
IF 2.1
Hong Shi,Tiantian Wang,Qian Zhao
Graphical In this study, we present a novel metal/sulfonic dual-acid based phosphotungstic acid ionic liquid catalyst for the ketone reaction of cyclohexanone with ethylene glycol. The ionic liquid was embedded into a B-SBA-16 carrier, and exhibited excellent catalytic properties and cycling stability. The conversion of cyclohexanone was 94.05 %, and the yield of ketal was 83.45 %. In recent years, ionic liquids have been widely used for industrial acid-catalysis. The enhancements of the acidity and immobilization of ionic liquids have been drawing increasing attention from researchers. In this study, dual-acid based phosphotungstic acid ionic liquids (PWILs) modified by a variety of metal ions (Fe 3+ , Cu 2+ , Al 3+ ) and sulfonic acid group (−SO 3 ) were synthesized. They were subsequently embeded into B-SBA-16 mesoporous molecular sieves with acidic sites to produce a plurality of encapsulating metal/sulfonic dual-acid based phosphotungstic acid ionic liquids (M n PWIL/B-SBA-16s) composite catalysts. The structural properties, thermal stability, and encapsulation of the as-fabricated composite catalysts were systematically investigated by FT-IR, BET, SAXD, TEM, TG-DSC and XPS. Moreover, the catalytic performances of the composite catalysts were evaluated using the ketalization of cyclohexanone with ethylene glycol as a model reaction. Among the different composite catalysts, Al 0.50 PWIL/B-SBA-16 showed the highest cyclohexanone conversion of 94.05 % and the maximum cyclohexanone glycol ketal yield of 83.45 %. Meanwhile, this catalyst still exhibited superior catalytic properties after five cycles of the catalytic reaction. These results demonstrate the high activity and durability of the novel ionic liquid composite catalyst.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 22
·9322-9334
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IF 9.8
Shi-Peng Chen,Jin-Long Zhu,Xing-Ru Chen,Zhi-Hao Wang,Yong-Jie Dan,Jing Wang,Sheng-Yang Zhou,Gan-Ji Zhong,Hua-Dong Huang,Zhong-Ming Li
The development of highly efficient and environmentally friendly solvents for dissolving cellulose, which is the most abundant natural polymer on Earth, remains a challenge, hindering its full utilization. Herein, a green protic ionic liquid, 1,1,3,3-tetramethylguanidinium methoxyacetate ([TMGH][MAA]), was found to exhibit attractive capacity to dissolve natural cellulose with an appropriate TMG/MAA molar ratio of 7 : 3 at 80 °C. The solubility of cotton linter and ultra-high molecular weight cotton fibers reached 13% (w/w) and 3% (w/w), respectively, surpassing that of most solvent systems currently used for the dissolution of cellulose. The experimental and simulation results verified that the excellent dissolution ability of [TMGH][MAA] for cellulose is mainly attributed to the destruction of the intrinsic hydrogen-bond networks in cellulose by the synergistic interactions of the [TMGH] cations and [MAA] anions with the hydroxyl groups in the cellulose chains, acting as highly efficient “intermolecular scissors”. The superiority of this novel dissolution system was further demonstrated by the remarkable comprehensive properties of the regenerated cellulose film including satisfactory thermostability, high transparency, and excellent mechanical properties. Furthermore, the satisfactory recovery performance of this solvent highlights its significant feasibility for large-scale industrial manufacturing. The proposed [TMGH][MAA] in this study exhibits great potential as a next-generation processing solvent for dissolving, and thus processing cellulose, promoting the sustainable development of high-value-added cellulose materials.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2023
·
IF 3.8
Hui Yu,Xiaojia Wu,Chuanqi Geng,Xinyu Li,Chencan Du,Zhiyong Zhou,Zhongqi Ren
The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry. In this study, a series of metal chloride–based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene (tetralin)/dodecane and tetralin/decalin systems were studied. Among these ionic liquids, 1-ethyl-3-methylimidazolium tetrachloroferrate ([EMIM][FeCl 4 ]) with the highest selectivity was used as the extractant. Density functional theory calculations showed that [EMIM][FeCl 4 ] interacted more strongly with tetralin than with dodecane and decalin. Energy decomposition analysis of [EMIM][FeCl 4 ]–tetralin indicated that electrostatics and dispersion played essential roles, and induction cannot be neglected. The van der Waals forces was a main effect in [EMIM][FeCl 4 ]–tetralin by independent gradient model analysis. The tetralin distribution coefficient and selectivity were 0.8 and 110, respectively, with 10% (mol) tetralin in the initial tetralin/dodecane system, and 0.67 and 19.5, respectively, with 10% (mol) tetralin in the initial tetralin/decalin system. The selectivity increased with decreasing alkyl chain length of the extractant. The influence of the extraction temperature, extractant dosage, and initial concentrations of the system components on the separation performance were studied. Recycling experiments showed that the regenerated [EMIM][FeCl 4 ] could be used repeatedly.
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Polymers
·
2023
·Vol. 16
·期 1
·103
·
IF 5
Qiao Zhou,Yuanyuan Zhao,Yafei Shi,Rongrong Zheng,Liying Guo
Utilizing triethylenediamine (DA), 1,3-propanesultone (PS), whose ring opens during the formation of the dizwiterion-intermediate DA-2PS, and the metal chlorides XCly, where X = Sn(IV), Zn(II),Al(III), Fe(III) and Mn(II), are used for the synthesis of five kinds of acidic metal-based functionalized ionic liquid catalysts ([DA-2PS][XCly]2). Their chemical structures, thermal stability and dual acidic active site were analyzed. We investigated the performance of [DA-2PS][XCly]2in catalyzing the esterification reaction between 2,5-furandicarboxylic acid (FDCA) and ethylene glycol (EG) to synthesize poly (ethylene 2,5-furandicarboxylate)(PEF). Among the catalysts tested, [DA-2PS][SnCl5]2exhibited the best catalytic performance under identical process parameters, and the optimal catalyst dosage was determined to be 0.05 mol% based on FDCA. The optimal conditions for the reaction were predicted using response surface methodology: a feed ratio of EG:FDCA = 1.96:1, an esterification temperature of 219.86 °C, a polycondensation temperature of 240.04 °C and a polycondensation time of 6.3 h, with a intrinsic viscosity of 0.67 dL·g−1. The resulting PEF was experimentally verified to exhibit an intrinsic viscosity of 0.68 dL·g−1and a number average molecular weight of 28,820 g·mol−1. Finally, the structure and thermal properties of PEF were characterized. The results confirmed that PEF possessed the correct structure, exhibited high thermal stability and demonstrated excellent thermal properties.
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ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Yin Hua Cui,Qing Shan Shi,Dan Dan Zhang,Ling Ling Wang,Jin Feng,Yi Wen Chen,Xiao Bao Xie
Ionic liquids (ILs), also known as green solvents, are widely acknowledged in several fields, such as chemical separation, synthesis, and electrochemistry , owing to their excellent physiochemical properties. However, their poor biodegradability may lead to environmental and health risks, posing a severe threat to humans, thus requiring further research. In this study, the biotoxicities of the imidazolium-based ILs were evaluated in Tetrahymena pyriformis . Moreover, IL detoxification was investigated by addition of glutathione (GSH), cysteine, and nicotinamide adenine dinucleotide (NADH). Reactive oxygen species (ROS) initiated by different IL types caused damage to Tetrahymena , while glutathione, cysteine, and NADH eliminated ROS, achieving the detoxification purposes. Detoxification results showed that NADH exhibited the best detoxification ability, followed by glutathione and cysteine. Finally, RT-PCR results suggested that metallothionein might have participated in IL detoxification.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Qingshan Liu,Jiamin Chu,Xiaoxi Yang,Yulu Huang,Mingxing Zhao,Qige Zheng,Yanxia Qi
The density of two functionalized ionic liquids (FILs) 1-methoxyethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide ([MOEmim][NTf 2 ] and 1-methoxyethyl-2,3-dimethylimidazolium bis[(trifluoromethyl)sulfonyl]imide [MOEmmim][NTf 2 ]) have been measured with ether solvents proprylene glycol monomethyl ether (PEGMME), diethylene glycol dimethyl ether (DEGDME), tetraethylene glycol dimethyl ether (TEGDME) at diluted concentration range. The determined temperature range is from 293.15 to 328.15 K at atmospheric pressure. The measured densities are used for the calculation of apparent molar volumes, V ϕ /m 3 ·mol −1 , at the temperature range. The effects of the ether ( O ) and methyl ( CH 3 ) introduction on imidazolium cation are discussed for the density and apparent molar volume in deeply. The Redlich-Rosenfeld-Meyer (RRM) equation was used for the fitting of apparent molar volumes, V ϕ /m 3 ·mol −1 , for the six studied dilute solutions. The infinite dilution apparent molar volumes, V ϕ /m 3 ·mol −1 , and limiting apparent molar expansibility, E Φ 0 / c m 3 · m o l - 1 · K - 1 , have been obtained and discussed from the RRM equation and polynomial equation. The thermal expansion coefficients, α/K −1 , have also been calculated and discussed from density for the studied dilute solutions in the temperature range.
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