AAPS PHARMSCITECH
·
2018
·Vol. 19
·期 5
·2288-2300
·
IF 2.666
Hu Beibei,Sun Wei,Yang Baixue,Li Heran,Zhou Liuchenzi,Li Sanming
Solvents, accounting the majority of the organogel system, have a tremendous impact on the characteristics of gels. To date, there is a large variety of organogel systems; relatively few have been investigated in the field of structure-solvent correlation. Here, a series of solvent parameters were applied to explore the role of solvent effect on network forming and gel property, intending to build the connection between the precise solvent parameter and gel property. Among the solvent parameters, Kamlet–Taft Parameters and Hansen solubility parameters can distinguish specific types of intermolecular interactions, which could correlate solvent parameter with the gel property. From an analysis of the morphologies obtained from POM and SEM, the gelator structure has an impact on its self-assembly. For possible conformations, the gelators were investigated through XRD. The investigation of solvent-property relationship will provide a theoretical basis for controllable drug delivery implants.
研究领域:
材料科学
·
药物递送
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Mengdan Ma,Anning Zhou,Tao Hong,Xinyu Jia,Moxuan Liu
Metal-organic frameworks (MOFs) are promising materials for CO 2 adsorption and capture. The unique crystal structure and the open porous structure of MOFs are key factors affecting their CO 2 adsorption performance, but the precise tuning of MOF structures remains a challenge. Herein, we applied the Kamlet-Taft method to investigate the effect of solvent proton-supplying/accepting capaity (β/α parameters) on the structure and CO 2 adsorption performance of Mg-MOF-74 by tuning the reaction solvent polarity. It was found that the ratio of the nucleation rate/growth rate of Mg-MOF-74 could be effectively controlled by adjusting the β/α value of the solvent, realizing the regulation of the crystal structure and morphology of Mg-MOF-74. In addition, the size of solvent molecules played a crucial role in the pore size of Mg-MOF-74. Interestingly, the solvent molecules were competitively coordinated with ligands and participate in the growth of Mg-MOF-74 upon decreasing the β/α value. The crystal structure, morphology and pore size of Mg-MOF-74 could be precisely regulated by the β/α value and molecular size of the reaction solvent, and the highest performing Mg-MOF-74 exhibited a CO 2 adsorption capacity of 7.38 mmol/g.
研究领域:
材料科学
·
环境化学
·
多孔材料
·
气体吸附
·
晶体工程
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Zhuo Liu,Cheng Li,Rongxin Zhang,Rude Lin,Zhaowen Dong,Bo Peng,Fan Zhang
Poly(bisphenol A carbonate) (PC) is a widely used engineering plastic that is often disposed of by landfilling or incineration, resulting in severe environmental concerns. Alcohol-aminolysis with ethanolamine can convert PC waste back into its monomer bisphenol A (BPA) and the valuable product 2-oxazolidinone. However, the use of hazardous solvents complicates both the recovery of PC and the synthesis and separation of 2-oxazolidinone. Herein, we developed a sustainable alcohol-aminolysis strategy utilizing the eco-friendly solvent ethanol (EtOH), achieving yields of 93% BPA and 88% 2-oxazolidinone from compact discs in 4 h at 80 °C. Multilinear regression revealed that elevated Kamlet–Taft parameters (β, π*) correlate strongly with enhanced PC alcohol-aminolysis efficiency for most solvents. Conversely, in monohydric alcohols, reactivity exhibits minimal dependence on β- and π*-values but is primarily governed by their steric hindrance. Mechanistic investigation reveals that EtOH enhances the nucleophilicity of ethanolamine, enabling nucleophilic attack on the activated carbonyl group of PC while facilitating cyclization of the intermediate. In gram-scale experiments, we recovered 8.64 g of BPA and 2.96 g of 2-oxazolidinone from 10.16 g of PC using simple filtration and evaporation. Economic assessments show that our innovative process presents a sustainable and economically viable method for upcycling waste polymers into valuable products, eliminating the need for hazardous solvents, harsh conditions, and complex purifications, thereby highlighting its potential for industrial applications.
研究领域:
高分子化学
·
绿色化学
·
废弃物管理
·
有机合成
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Yuling Zhang,Hongwei Ren,Baochai Li,Syarah Mat Udin,Hasmerya Maarof,Wen Zhou,Fengfei Cheng,Jiaoruo Yang,Yize Liu,Hajar Alias,Erhong Duan
Deep eutectic solvents (DESs) composed by amino acids (L-arginine, L-proline, L-alanine) as the hydrogen bond acceptors (HBAs) and carboxylic acids (formic acid, acetic acid, lactic acid, levulinic acid) as hydrogen bond donors (HBDs) were prepared and used for the dissolution of dealkaline lignin (DAL). The mechanism of lignin dissolution in DESs was explored at molecular level by combining the analysis of Kamlet-Taft (K-T) solvatochromic parameters, FTIR spectrum and density functional theory (DFT) calculations of DESs. Firstly, it was found that the formation of new hydrogen bonds between lignin and DESs mainly drove the dissolution of lignin, which were accompanied by the erosion of hydrogen bond networks in both lignin and DESs. The nature of hydrogen bond network within DESs was fundamentally determined by the type and number of functional groups in both HBA and HBD, which affected its ability to form hydrogen bond with lignin. One hydroxyl group and carboxyl group in HBDs provided active protons, which facilitated proton-catalyzed cleavage of β-O-4, thus enhancing the dissolution of DESs. The superfluous functional group resulted in more extensive and stronger hydrogen bond network in the DESs, thus decreasing the lignin dissolving ability. Moreover, it was found that lignin solubility had a closed positive correlation with the subtraction value of α and β (net hydrogen donating ability) of DESs. Among all the investigated DESs, L-alanine/formic acid (1:3) with the strong hydrogen-bond donating ability (acidity), weak hydrogen-bond accepting ability (basicity) and small steric-hindrance effect showed the best lignin dissolving ability (23.99 wt%, 60 °C). On top of that, the value of α and β of L-proline/carboxylic acids DESs showed some positive correlation with the global electrostatic potential (ESP) maxima and minima of the corresponding DESs respectively, indicating the analysis of ESP quantitative distributions of DESs could be an effective tool for DESs screening and design for lignin dissolution as well as other applications.
研究领域:
化学
·
材料科学
·
生物技术
·
可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Weimeng Cai,Haojie Du,Erju Wang,Yuting Qiang,Kunhong Hu,Jianhua Guo
The synthesis of value-added chemicals from renewable biomass is becoming increasingly important in the transition to a sustainable and low-carbon energy system. Herein, we demonstrate a solvent-polarity modulation strategy to engineer biomass-derived Cu-MOF using 2,5-furandicarboxylic acid (FDCA) as a renewable ligand, where tailored β/α ratios via Kamlet-Taft parameters balance nucleation-growth kinetics to optimize textural properties. Pyrolyzed Cu-MOF at 500 °C under a nitrogen atmosphere yield the Cu/C catalysts, which were subsequently employed in the selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Among the various solvents used, the Cu-MOF precursor synthesized in a mixed solvent of methanol and N, N-dimethylformamide (DMF) demonstrated the highest catalytic performance, outperforming those synthesized in other solvents. This highlights the significant impact of solvent selection on the structure of Cu-MOF, which in turn affects their hydrogenation activity. Advanced characterization confirming that the uniform Cu dispersion (confirmed by HRTEM mapping) and Cu⁰/Cu⁺ electronic synergy (via Cu Auger analysis) enhanced hydrogenation performance. Additionally, the biomass-derived catalysts exhibited excellent durability. Overall, this research provides a promising approach to develop highly efficient catalysts using renewable ligands and demonstrates the potential of regulating catalyst properties through the strategic selection of solvents, as informed by Kamlet-Taft parameters.
研究领域:
催化化学
·
绿色化学
·
材料科学
·
可再生能源
·
化学合成
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Jian-Dong Wang,Qi Gu,Zi-Hui Cai,Guo-Sheng Liu,Quan Zhou,Li-Na Fu,Shi-Liang Yang,Su Zhang,Yujie Fu
In this study, a green CO2-responsive switchable hydrophilic solvent (SHS) was screened in the strategy of extracting and enriching active components with different polarities from a plant matrix. The mechanism of solvent switching was confirmed by Fourier transform infrared spectroscopy (FT-IR) and nuclear magnetic resonance (NMR) spectroscopy. Furthermore, the function of SHS polarity switching was proven by Kamlet–Taft parameters, and the polarity parameter π* of the solvent increased from 0.34 to 1.01 after introducing CO2. The solvent system was used to extract the active ingredients from Rosa roxburghii; a series of single factor experiments were conducted using the Box-Behnken design in order to optimize the process. In addition, the phenomenon of the SHS/water two-phase system being heated by ultrasound to produce an O/W micellar system was observed, which provided solvent solubilization. Moreover, after 5 cycles, the solvent still ensured a high extraction capacity of the target components. In addition, density functional theory (DFT) and molecular dynamics theory revealed that van der Waals forces and hydrogen bonding made the SHS more biocompatible with the target compounds and that van der Waals forces played a significant impact. In conclusion, the current process offered an ecologically acceptable, promising, and long-term alternative approach for simultaneously extracting and enriching hydrophilic and hydrophobic phytochemicals from plant materials.
研究领域:
植物化学
·
绿色化学
·
分析化学
·
溶剂科学
·
超声波技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Guanhua Wang,Xiaoqian Liu,Bo Yang,Chuanling Si,Ashak Mahmud Parvez,Jinmyung Jang,Yonghao Ni
Lignin heterogeneity, involving complex structure and high polydispersity, is a key challenge that restricts its value-added applications. Fractionation of heterogeneous lignin into several homogeneous subdivisions is an attractive and practical strategy to overcome this limitation. In this work, γ-valerolactone (GVL), a sugar-derived product, was used as a green solvent for lignin fractionation when mixed with water. The enzymatic hydrolysis lignin (EHL) was subdivided into three different fractions (F1, F2, and F3) by dissolving it completely in 60% aqueous GVL and then following gradient precipitation in 40%, 30%, and 5% aqueous GVL solutions, sequentially. Detailed characterization techniques were conducted to provide a comprehensive evaluation of the three obtained lignin fractions. Moreover, the proposed fractionation mechanism was further investigated on the basis of Kamlet–Taft parameters. The gel permeation chromatography (GPC) analyses showed that the three fractions presented lower polydispersity than the parent EHL and, furthermore, a gradual decreasing molecular weight due to the different solubility of various molecular weight lignins in aqueous GVL solvents. The structural analyses revealed that with the decrease of molecular weight, the guaiacyl unit content in lignin fractions decreased, with significant increases of functional groups (i.e., aromatic/aliphatic hydroxyl and carboxyl groups). The solvent recycling study showed that the aqueous GVL had a high recovery, and the recycled GVL had the same lignin fractionation performance as fresh GVL. Overall, compared with traditional fractionation using multiple organic solvents, the present work provides a green and efficient route to fractionate lignin and, therefore, significantly decreases its molecular weight polydispersity and structural heterogeneity.
研究领域:
化学工程
·
材料科学
·
绿色化学
·
生物技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2019
·
IF 2.29
Yameng Wan,Rui Zhao,Pengshuai Zhang,Haixia He,Jiao Sha,Tao Li,Baozeng Ren
Solubility of ( R )-(-)-phenylephrine hydrochloride ( R -PEHC) in ten pure solvents including methanol (MtOH), ethanol (EtOH), n -propanol (NPrOH), iso-propanol (IPrOH), 2-methoxyethanol, 2-ethoxyethanol, 2-propoxyethanol, 2-butoxyethanol, N-methyl pyrrolidone (NMP) and N,N-dimethylformamide (DMF) was determined by using a laser monitoring technique in the range of 278.15 K to 323.15 K under 0.1 MPa. Solubility of R -PEHC increases with the increment of temperature. The solvent effect on R -PEHC solubility was investigated by the linear solvation energy relationships concept (Kamlet-Taft parameters). The interaction energy ( E inter ) between R -PEHC and selected solvents was calculated by molecular simulation to explain the solubility behavior. Experimental solubility was correlated by five activity coefficient models including the Two-Suffix Margules model, Wilson model, NRTL model, NRTL-SAC model and uniquac model. Five models can fit experimental solubility values well. Furthermore, thermodynamic properties of solutions of R -PEHC in selected solvents were investigated by the van’t Hoff equation.
研究领域:
物理化学
·
热力学
·
药学
·
分子模拟
✓ 已验证
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Yanjun Chen,Junqiang Shan,Yulian Cao,Xin Shen,Chenglun Tang,Ming Li,Wei Zhuang,Chenjie Zhu,Hanjie Ying
Mechanocatalytic depolymerization of lignocellulose constitutes a new frontier in biorefinery. In this study, a weak alkali-oxidation pretreatment with sodium percarbonate was employed to isolate hemicellulose from corncob, which was comprehensively characterized by FTIR, 1 H, 13 C, and 2D HSQC NMR. The influences of impregnation solvent, the type and dosage of acid catalyst, and ball-milling time on the mechanocatalytic depolymerization of hemicellulose have been systematically investigated. A mathematical model based on Kamlet-Taft parameters was first proposed to reveal the relationship between the reaction conversion and the solvent properties, and the results suggested a solvent possessing a high polarity/polarizability and Lewis basicity is favorable for the reaction. Under the optimal conditions, 97.1% conversion of hemicellulose with 93.1% selectivity of xylooligosaccharides based on xylans could be achieved within 2 h. Qualitative high-resolution ESI-MS and quantitative HPAEC analysis demonstrated the good solubility of the obtained xylooligosaccharides was ascribed to the depolymerization of hemicellulose rather than the formation of sulfonated oligosaccharides .
研究领域:
生物炼制
·
化学工程
·
分析化学
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
FLUID PHASE EQUILIBRIA
·
2019
·
IF 2.514
Yameng Wan,Haixia He,Pengshuai Zhang,Rui Zhao,Jiao Sha,Tao Li,Baozeng Ren
Mole-fraction solubility of 5-norbornene-2,3-dicarboximide (NODI) in eleven solvents including methanol (MtOH), ethanol (EtOH), 2-ethoxyethanol, methyl acetate (MAC), ethyl acetate (EAC), n-propyl acetate (NPAC), isopropyl acetate (IPAC), n-butyl acetate (NBAC), acetone (DMK), N,N-dimethylformamide (DMF) at (278.15–323.15) K and 1,4-dioxane at (288.15–323.15) K was experimentally measured by laser monitoring technique under 0.1 MPa. Solubility of NODI increased with the increasing temperature. Hansen Solubility Parameter was employed to explain the solubility behavior. The Kamlet-Taft parameters were calculated to investigate the solvent effect based on linear solvation energy relationships concept. Thermodynamic modeling including the Two-Suffix Margules model, Wilson model, NRTL model, NRTL-SAC model and UNIQUAC model were employed to correlate the experimental solubility. Wilson model and NRTL-SAC model were more suitable in correlation with solubility data. Furthermore, thermodynamic properties of mixing process (Δ mix G , Δ mix H , Δ mix S , ln γ 1 ∞ , H 1 E,∞ , ζ TS and ζ H ) were discussed based on Wilson equation.
研究领域:
化学工程
·
物理化学
·
热力学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Fahui Li,Yiyue Shen,Yupei Deng,Jingchun Zhang,Qiqi Wang,Haoyuan Chen,Mai Ouyang,Qianwen Jiang,Guowei Wang,Linghua Zhuang
Ionic liquids (ILs) have emerged as a promising class of green solvents suitable for cellulose dissolution. In this study, two dihydroxyl-functionalized ionic liquids, 1-methyl-3-(2,3-dihydroxypropyl)-imidazolium chloride ([DPmim]Cl) and 1-butyl-3-(2,3-dihydroxypropyl)-imidazolium chloride ([DPbim]Cl), were prepared for microcrystalline cellulose (MCC) dissolution. The physical properties of [DPmim]Cl and [DPbim]Cl, such as relative viscosity, density, electrical conductivity, and Kamlet-Taft parameters (β and π*), were evaluated. The dissolution and regeneration properties of MCC in [DPmim]Cl and [DPbim]Cl were investigated. The regenerated MCC was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), and X-ray diffraction (XRD). Density functional theory (DFT) simulations were used to investigate the interactions between ionic liquid and cellobiose. [DPmim]Cl and [DPbim]Cl, with higher β-values (0.975 and 1.098) respectively, exhibited stronger hydrogen bonding alkalinity. This increased alkalinity enhanced their ability to accept hydrogen bonds from cellulose, which in turn weakened the inter- and intra-molecular hydrogen bonds within cellulose. As a result, the dissolution of MCC was promoted. The dissolution of MCC in [DPmim]Cl was faster than [DPbim]Cl at same temperature. FTIR, TGA, and XRD characterizations showed that the hydrogen bonding network of microcrystalline cellulose was disrupted during ionic liquid dissolution. DFT simulations unveiled the formation of strong hydrogen bonds between the hydroxyl groups of ILs and the hydroxyl or ether linkages in cellulose. These hydrogen bonds have been identified as a potential crucial factor in facilitating the dissolution of cellulose.
研究领域:
化学
·
材料科学
·
物理化学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）