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Nanoscale Research Letters · 2019 ·Vol. 14 ·期 1 ·1-7 · IF 3.159

Synergistic Exfoliation of MoS2 by Ultrasound Sonication in a Supercritical Fluid Based Complex Solvent

Tan Xi,Kang Wenbin,Liu Jingfeng,Zhang Chuhong

Molybdenum disulfide (MoS 2 ) is an extremely intriguing low-D layered material due to its exotic electronic, optical, and mechanical properties, which could be well exploited for numerous applications to energy storage, sensing, and catalysis, etc., provided a sufficiently low number of layers is achieved. A facile exfoliation strategy that leads to the production of few-layered MoS 2 is proposed wherein the exfoliation efficacy could be synergistically boosted to > 90% by exploiting ultrasound sonication in supercritical CO 2 in conjunction with N -methyl-2-pyrrolidone (NMP) as the intercalating solvent, which is superior to general practiced liquid exfoliation methods wherein only the supernatant is collected to avoid the majority of unexfoliated sediments. The facile and fast exfoliation technique suggests an exciting and feasible solution for scalable production of few-layered MoS 2 and establishes a platform that contributes to fulfilling the full potential of this versatile two-dimensional material.

CAS / MDL: 872-50-4 1317-33-5
研究领域: 材料科学 · 化学工程 · 纳米技术
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2017 · IF 2.323

Measurement and Correlation of Vapor–Liquid Equilibrium for R124 (1-Chloro-1,2,2,2-Tetrafluoroethane)-NMP (N-Methyl-2-Pyrrolidone) and R124-DMF (N,N-Dimethylformamide) Mixtures

Shiming Xu,Wei Wang,Xi Wu,Jungyong Hu,Mengnan Jiang

Vapor–liquid equilibrium data of binary working pairs play a crucial part in the research of absorption process and absorption refrigeration technology. In this paper, the VLE data of binary mixtures, R124-NMP and R124-DMF, were measured in a temperature range from 303.15 to 363.15 K, using a VLE measurement apparatus. The activity coefficient model of five-parameter nonrandom two liquid (NRTL) was selected to correlate all the VLE data acquired by measurement. The maximum relative deviation of the pressure between the measurement data and calculated data for R124-NMP and R124-DMF were 3.80% and 3.27% respectively, and the average relative deviation of the pressure were 1.25% and 1.17% respectively. The correlated results coincide well with the measurement data and show that the VLE characteristics of R124-NMP and R124-DMF mixtures have a negative deviation from Raoul’s law. Comparing three absorbents, DMF, DMAC and NMP, the activity coefficient of R124 in DMF is largest, that in DMAC is second, and that in NMP is smallest.

研究领域: 热力学 · 制冷与空调 · 化学工程
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INTERNATIONAL JOURNAL OF PHARMACEUTICS · 2023 · IF 5.8

In situ formation of injectable organogels for punctal occlusion and sustained release of therapeutics: design, preparation, in vitro and in vivo evaluation

Ziqin Cao,Yangnan Chen,Shaoyun Bai,Zhiyun Zheng,Yan Liu,Shuangying Gui,Shuang Shan,Jiabao Wu,Ning He

The treatment of dry eye mainly includes instillation of cyclosporine A (CsA) nanoemulsion or the use of punctal plugs. Therefore, in this study, a novel injectable in situ organogel plug was developed using CsA as a model drug, stearic acid , injectable soybean oil, and N -methyl-2-pyrrolidinone (NMP) (1.25:10:0.6, w/v/v) as gel materials, to provide a dual mechanism for dry eye treatment. The formulated CsA injectable in situ organogel (CsA-OG) was evaluated in terms of stability, in vitro release, rheology, ocular irritation, punctal occlusion tests, and ocular distribution assessment. In vivo ocular distribution investigations showed that CsA-OG achieved considerably higher C max (1.94, 1.92 and 1.97-fold respectively) and AUC 0-72h in the cornea, conjunctiva, and sclera (2.49, 2.27 and 2.15-fold respectively) than ciclosporin eye drops ( p  < 0.05). In vitro model evaluation demonstrated significant decrease in flow flux to 52.78 % at 2 min after CsA-OG injection. According to evaluation of the in vivo model, the organogel plug can completely block the lacrimal passages and greatly decrease the lacrimal drainage rate ( p  < 0.05). The above results suggest that these intracanalicular CsA-OG plugs can offer more extensive clinical applications than existing lacrimal drainage plugs and may act as a drug delivery system .

研究领域: 药剂学 · 药物递送系统 · 眼科学
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JOURNAL OF ORGANIC CHEMISTRY · 2023 · IF 3.6

Scalable Palladium-Catalyzed Alkoxycarbonylation of Conjugated Dienes

Zi-Heng Zhang,Li-Jun Han,Shuang-Shuang Ma,Yi-Ran Du,Zheng-Kun Yu,Jin-Qing Lin,Bao-Hua Xu

The Pd(cod)Cl2-catalyzed alkoxycarbonylation of conjugated dienes to β,γ-unsaturated esters was approached by both intramolecular phosphinesulfonate L1 and intermolecular PPh3/PTSA in this study. However, the poor solubility of the Pd/L1 complex and the labile monodentate Pd/PPh3 structure restricts the system efficiency, especially for the scale-up application. By contrast, the stable and well-soluble bidentate Xantphos system allows for the quantitative formation of 3-pentenoate (96%) on a gram scale within 6 h in weakly alkaline N-methylpyrrolidone (NMP), which also functions as a basic site to promote the rate-limiting alcoholysis step while reducing the dosage of ligand to a theoretical value.

研究领域: 有机化学 · 催化 · 合成化学
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

A novel organic solvent ultrafiltration membrane of polyimide/polyethyleneimine@TiO2 with high solvent permeability

Ni-Jie Liu,Jun-Yan Yu,Xing-Yu Chen,Li-Fen Liu

Organic solvent ultrafiltration (OSU) membrane as the crucial supporting layer of thin-film composite (TFC) organic solvent nanofiltration (OSN) membrane can help the OSN technology to satisfy the rapidly growing demand for small-molecular separation and purification in organic solvent systems. Aiming at the two main bottlenecks of poor tolerance to strong polar solvents and low solvent flux of the conventional commercial polyimide (PI) ultrafiltration (UF) membrane, in this study, a facile method was proposed to prepare a novel polyimide/polyethyleneimine@TiO2 (PI/PEI@TiO2) OSU membrane with improved solvent resistance and permeability by synchronously coupling the non-solvent-induced phase transformation (NIPs), chemical crosslinking and interfacial in-situ biomineralization. Dut to the chemical crosslinking between PEI and PI, the PI/PEI@TiO2 membrane exhibited good resistance to more organic solvents including the strong polar aprotic solvents (e.g., DMF, NMP and DMSO), ordinary polar solvents (e.g., ethanol) and nonpolar solvents (e.g., n-hexane). At the same time, PEI synchronously catalyzed Ti-BALDH to in-situ generate the TiO2 nanoparticles via interfacial biomineralization, which improved the solvent flux of the PI/PEI@TiO2 membrane due to the creation of more channels and promoted the compatibility of TiO2 within PI/PEI matrix. Especially, the PI/PEI@TiO2-5 membrane with 5 wt% TiO2 loading showed the optimal solvent resistance and high flux in strong polar aprotic solvents (>50 L m−2 h−1·bar −1 in DMF). Therefore, the resultant new PI/PEI@TiO 2 OSU membrane will have a promising separation application in the organic solvent systems in the future.

研究领域: 材料科学 · 化学工程 · 膜技术
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

One-Pot Synthesis of Dimethyl Hexane-1,6-diyldicarbamate from CO2, Methanol, and Diamine over CeO2 Catalysts: A Route to an Isocyanate-Free Feedstock for Polyurethanes

Kirill A. Alferov,Zhongwei Fu,Shuxian Ye,Dongmei Han,Shuanjin Wang,Min Xiao,Yuezhong Meng

A new one-pot synthesis method of dimethyl hexane-1,6-diyldicarbamate (HDC), a potential intermediate compound in the synthesis of polyurethanes, from CO2, methanol, and 1,6-hexanediamine (HDA) is disclosed. The starting materials are renewable, stable, easily available, and cheap. The process was implemented in 1-methyl-2-pyrrolidinone (NMP) solvent over CeO2 catalysts. Three different CeO2 catalysts (commercial nanospheres, CeO2(c) obtained by direct calcination of (NH4)2Ce(NO3)6, and CeO2 nanorods) were tested in this reaction and their micromorphology and physical–chemical properties were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), and N2 adsorption. CeO2 nanorods proved to be the most active catalytic material. The influence of different parameters on reaction outcome was studied. The yield of HDC was about 80% under optimized reaction conditions. Experiments for better understanding of reaction mechanism were also performed.

研究领域: 化学工程 · 催化 · 材料科学 · 有机化学 · 可持续化学
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GIANT · 2023 · IF 7

Hydrogen-bonding polymer complexation: Coacervation interfered with gelation

Caihong Zhang,Weijie Wang,Pengfei Zhang,Shuguang Yang

Complexation between polymers of different species in a common solvent is a fundamental process in various applications such as functional polymeric membrane and drug delivery, yet the understanding of energetics, phase behaviors, and kinetics of polymer complexation is rather challenging partially due to the multi-component nature of the system. In this work, we investigate the hydrogen-bonding complexation of poly(acrylic acid) (PAA) and poly(vinylpyrrolidone) (PVPON) in different solvents, and identify a variety of phase states, including homogenous solution, solid precipitate, liquid–liquid separation, gelation, and kinetically trapped structures. Among different solvents, N -methyl-2-pyrrolidone (NMP) has a similar structure to the repeating unit of PVPON and the complexation in NMP almost has no heat, suggesting the process is driven by entropy. The PAA/PVPON-NMP system exhibits an upper critical solution temperature; specifically, as the temperature decreases, a homogeneous solution first becomes opalescent, then undergoes a liquid–liquid separation, and finally undergoes a liquid–gel separation. On the other hand, when the polymer concentration is above a threshold, a homogenous solution turns into a gel directly without involving liquid–liquid separation with decreasing temperature. Accordingly, we construct a temperature–concentration phase diagram that shows how the gelation interplays with coacervation. This work provides a broad vision on phase behaviors of polymer complexation.

CAS / MDL: 9003-01-4
研究领域: 高分子科学 · 材料科学 · 物理化学
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CHEMICAL PAPERS · 2016 ·Vol. 70 ·期 5 ·585-593 · IF 1.326

Liquid—liquid equilibria of ternary systems of 1-hexene/hexane and extraction solvents

Lin Zhu,Fang-Fang Li,Ji-Qin Zhu,Zhi-Gang Lei

Olefins and paraffins are important basic chemical raw materials with so similar molecular structure and volatility that their separation is a difficult and energy-consuming process. Liquid–liquid equilibrium (LLE) data were determined for ternary systems of: 1-hexene + hexane + solvent at 25°C, 30°C, and 35°C, and N-formylmorpholine (NFM), N-methyl-2-pyrrolidone (NMP), 7-butyrolactone (GBL), and 1-methylimidazole (1-MEI) as the solvents studied. Liquid–liquid equilibrium data for each system were correlated to the NRTL (Non-Random Two Liquid) equation and the interaction parameters presented. The calculated results agree well with the experimental data.

研究领域: 化学工程 · 物理化学
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Nature Energy · 2025 · IF 60.1

Solvated-intermediate-driven surface transformation of lead halide perovskites

Liu Sanwan,Miao Tianyin,Wang Jianan,Zhang Yong,Chen Rui,Lei Xia,Qin Wenming,Zhu Zhongjie,Lu Lanlu,Chen Zhenhua,Cui Peng,Li Liang,Li Meicheng,Xu Erxiang,Shen Yang,Cho Seong Chan,Lee Sang Uck,Cho Seong-Ho,Liu Zonghao,Chen Wei,Park Nam-Gyu

The certified quasi-steady-state efficiency of reported inverted perovskite solar cells (PSCs) has rarely surpassed 26%, primarily attributed to interfacial energy-level misalignment and defect-mediated non-radiative recombination. Here we report a surface-phase-transformation strategy of introducing a minuscule amount of N -methyl pyrrolidone (NMP) into the piperazinium diiodide (PDI)-dissolved isopropanol solution to mitigate these challenges. We demonstrate that NMP induces a distinct crystallization pathway on perovskite surfaces during the post-treatment stage, transitioning from a solvated intermediate phase to the α-phase perovskite, bypassing the conventional δ-intermediate-phase → α-phase route, which improves the crystallinity of perovskite surfaces and reduces contact losses. Moreover, NMP enhances the interaction between PDI and perovskites, further optimizing interfacial band alignment. Consequently, we demonstrate high certified power conversion efficiencies of 26.87% (stabilized efficiency), 23.00% and 29.08% for single-junction PSCs, mini-modules and all-perovskite tandems, respectively. Maximum-power-point tracking retains 96% of initial efficiency after 2,500 h under 1-sun illumination at 65 °C in ambient air.

CAS / MDL: 110-60-1 7440-23-5
研究领域: 光伏技术 · 材料科学 · 可再生能源 · 半导体物理 · 纳米技术
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Polymer Chemistry · 2020 ·Vol. 12 ·期 4 ·526-533 · IF 5.342

Novel tetraphenylethylene (TPE)-functionalized nitroxide/alkoxyamine for nitroxide-mediated homogeneous and heterogeneous polymerizations

Huanhuan Ma,Linan Wang,Yachao Liang,Zhe Cui,Peng Fu,Minying Liu,Xiaoguang Qiao,Xinchang Pang

Tetraphenylethylene (TPE)-containing 4-amino-2,2,6,6-tetramethylpiperidine-1-oxyl (NH2-TEMPO) and 3-(((2-cyanopropan-2-yl)oxy)(cyclohexyl)amino)-2,2-dimethyl-3-phenylpropanenitrile (Dispolreg 007) were synthesized and utilized to mediate/initiate NMP in both homogeneous and heterogeneous polymerization systems. The introduction of TPE groups decreased the C–O bond dissociation energy (BDE) of NH2-TEMPO-St and led to more efficient NMP with a higher reaction rate, even at lower temperatures. Moreover, for both solution polymerization and miniemulsion polymerization, quantitative information of the polymerization process could be easily acquired with the naked eye without destroying the reaction system, by building the relationship between the increased photoluminescence (PL) intensity of the system and monomer conversion as well as the molecular weight (Mn).

研究领域: 高分子化学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Fluorine incorporation for enhancing solvent resistance of organic solvent nanofiltration membrane

Yi Guo,Shuxuan Li,Baowei Su,Bishnupada Mandal

The solvent resistance performance of organic solvent nanofiltration (OSN) membranes still need to improve for their applications in harsh organic environments. We envisioned that fluorine (F) atoms could enhance the solvent resistance of OSN membranes owing to the high bond energy of C-F bonds. Herein, a kind of novel solvent-resistant F-containing OSN membranes was successfully prepared via interfacial polymerization (IP), chemical crosslinking and solvent activation processes. Mixtures of m-phenylenediamine (MPD) and 5-(trifluoromethyl)-1,3-phenylenediamine (TFMPD) were used as aqueous monomers, and trimesoyl chloride (TMC) was used as an organic monomer. The incorporation of F-containing monomer is proved useful to regulate the surface morphology and the roughness of the OSN membranes. Two folds increase in permeance for ethanol (achieving 41.6 L m −2  h −1  MPa −1 ) and a rejection of 99.4% for Rhodamine B (479 Da) were achieved at optimal F-containing monomer ratio. Three persistent static immersion tests, in NMP for 90 days (room temperature), in NMP for 10 days (80 °C), and in DMF for 31 days (80 °C), respectively, and one continuous cross-flow filtration test for 104 h using Rose Bengal (1017 Da)/DMF solution at room temperature demonstrated that the prepared OSN membranes owned an outstanding solvent resistance, proving vast potential in organic solvent separation and purification.

CAS / MDL: 368-53-6
研究领域: 材料科学 · 化学工程 · 膜技术
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JOURNAL OF POLYMER RESEARCH · 2023 ·Vol. 30 ·期 9 ·1-8 · IF 2.8

Preparation of PDMS STEM gels through oxygen tolerance nitroxide mediated polymerization

Qiao Xiaoguang,Dong Xin,shi Ge,He Yanjie,Pang Xinchang

The postsynthesis polymeric modifications by grafting from the active sites were the primary focus of the structurally tailored and engineered macromolecular (STEM) gels. Therefore, Reversible-deactivation radical polymerization (RDRP) techniques have been employed to more precisely tailor and tune STEM gels. In contrast to atom transfer radical polymerization (ATRP) and reversible addition-fragmentation chain transfer polymerization (RAFT), nitroxide-mediated polymerization (NMP) is known to have the advantages of simple components and pure products. Here we report the preparation of polydimethylsiloxane (PDMS) composite gel networks through oxygen tolerance NMP process, with tert-Butyl acrylate (tBA) and fluorinated monomer 2-(Perfluorooctyl)ethyl methacrylate (FMA) as functional comonomers. Compared with conventional radical polymerization (FRP) method, composite gels prepared through NMP method showed higher swelling rate and elongation at break, which proved that the network structure formed by NMP was more uniform. In addition to better thermal stability and toughness, the dormant polymer chain could be reactivated and lead to the “living” post-modification of PDMS gel matrix.

研究领域: 材料科学 · 高分子化学 · 材料工程
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