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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2020 ·Vol. 95 ·期 8 ·2195-2207 · IF 2.75

Preparation of a novel hydrophobic interaction chromatography with higher selectivity by introducing spatial recognition

Wei Shi,Si-Qi Zhang,Kai-Bin Li,Ye-Jing Deng,Chen-Yi Wang,Yi-Ting Lu,Jiao-Jiao Liu,De-Man Han

BACKGROUND Hydrophobic interaction chromatography (HIC), as a typical separation technology, often suffers from low selectivity because it has a single interaction mode. Herein, a novel HIC resin (Octyl@BSA) with imprinted layer was synthesized and used for protein adsorption. Bovine serum albumin (BSA) and bovine serum γ-globulin (bIgG) were used as model competitive proteins in this study. The effects of pH, salt type, concentration, and mass ratio were then investigated. RESULTS The data from the static and dynamic adsorption experiments indicated that the introduction of spatial recognition effectively reduced the adsorption of competitive proteins, leading to significant improvements in selectivity. In comparison with raw HIC resin, Octyl@BSA retained a high binding capacity for BSA but rejected other proteins through spatial recognition. The maximum selectivity factors ( α ) of this resin may be close to 5. The adsorption kinetics and frontal adsorption experiments further confirmed the improvement in selectivity in batch and column mode. In addition, the recyclability of Octyl@BSA was tested using ten continuous BSA adsorption–desorption cycles. CONCLUSION This study demonstrated that the introduction of spatial recognition was an effective strategy for enhancing the advantage of target proteins during competitive adsorption, leading to an improvement in selectivity for HIC. © 2020 Society of Chemical Industry

研究领域: 生物化学 · 分离技术
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JOURNAL OF CHROMATOGRAPHY A · 2014 · IF 4.258

Influence of the crosslinker type on the chromatographic properties of hydrophilic sulfoalkylbetaine-type monolithic columns

Chusheng Liu,Weijia Chen,Guangxin Yuan,Yao Xiao,Jacques Crommen,Shihai Xu,Zhengjin Jiang

In order to investigate the effects of the crosslinker on the separation performance of polar zwitterionic sulfoalkylbetaine-type monolithic columns, three crosslinkers, i.e. 1,4-bis(acryloyl)piperazine (PDA), ethylene dimethacrylate (EDMA) and N , N ′-methylenebisacrylamide (MBA), were copolymerized with the hydrophilic monomer N , N -dimethyl- N -acryloyloxyethyl- N -(3-sulfopropyl)ammonium betaine (SPDA). The chromatographic properties of the three hydrophilic sulfoalkylbetaine-type monolithic columns, including column efficiency, permeability, porosity and separation mechanism, were systematically compared using scanning electron microscopy or micro-HPLC. Good selectivity in micro-HPLC separations was achieved on all three monolithic columns. The results indicate that the polarity of sulfoalkylbetaine-type monolithic columns may be related to the polarity of the crosslinker, which further affects column selectivity and efficiency. A particularly high column efficiency (100,000 plates/m) was obtained on the novel poly(SPDA- co -PDA) monolithic column at a linear velocity of 1   mm/s using thiourea as test analyte. A higher resolution was also observed for nucleobases, nucleosides and hydrophilic organic acids on this novel poly(SPDA- co -PDA) monolithic column compared to the other two columns.

研究领域: 分析化学 · 色谱技术
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2018 · IF 3.141

Role of Hydrophobic Interaction in Driving the Partitioning of Metal Ions in a PEG-Based Aqueous Two-Phase System

Pan Sun,Kun Huang,Jieyuan Lin,Huizhou Liu

PEG-based aqueous two-phase systems (ATPS) for extraction and removal of metal ions from industrial wastewaters is a promising strategy to replace traditional organic-aqueous two phase systems, due to its environmentally friendly advantages and excellent separation efficiency from controllable phase structure and physicochemical properties. However, controversy still remains about the partitioning mechanism of metal ions into the PEG-rich phase in ATPS. The present contribution revealed that a specific hydrophobic interaction was a main driving force for the transferring of Cr(VI) ions into the PEG-rich phase in ATPS. The properties of aqueous media around the PEG molecules and Cr(VI) ions also played a crucial role in the partitioning of Cr(VI) ions in the PEG-base ATPS. The PEG-rich phase in the ATPS exhibited a specific affinity toward poorly hydrated HCrO4– ions, compared to the strongly hydrated CrO42– ions. The difference in the properties of aqueous media in the coexisting liquid phases was response for the partitioning of Cr(VI) ions in the PEG-base ATPS. It was confirmed by combined application of UV–vis spectroscopy and molecular dynamics simulations. The present work provides a new understanding into the microscopic mechanism of the partitioning of metal ions in the polymer-based ATPS.

CAS / MDL: 10034-82-9
研究领域: 环境科学 · 化学
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Materials · 2015 ·Vol. 8 ·期 12 ·8701-8713 · IF 2.651

Acid Denaturation Inducing Self-Assembly of Curcumin-Loaded Hemoglobin Nanoparticles

Kaikai Wang,Juan Wang,Wenwen Hu,Yifan Zhang,Feng Zhi,Zaigang Zhou,Jinhui Wu,Yiqiao Hu

Hemoglobin is a promising drug carrier but lacks extensive investigation. The chemical conjugation of hemoglobin and drugs is costly and complex, so we have developed curcumin-loaded hemoglobin nanoparticles (CCM-Hb-NPs) via self-assembly for the first time. Using the acid-denaturing method, we avoid introducing denaturants and organic solvents. The nanoparticles are stable with uniform size. We have conducted a series of experiments to examine the interaction of hemoglobin and CCM, including hydrophobic characterization, SDS-PAGE. These experiments substantiate that this self-assembly process is mainly driven by hydrophobic forces. Our nanoparticles achieve much higher cell uptake efficiency and cytotoxicity than free CCM solutionin vitro. The uptake inhibition experiments also demonstrate that our nanoparticles were incorporated via the classic clathrin-mediated endocytosis pathway. These results indicate that hemoglobin nanoparticles formed by self-assembly are a promising drug delivery system for cancer therapy.Keywords:drug carrier;hydrophobic forces;self-assemble;cell uptake

CAS / MDL: 61791-12-6
研究领域: 生物化学 · 药剂学 · 肿瘤学
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MICROCHIMICA ACTA · 2017 ·Vol. 184 ·期 8 ·2629-2636 · IF 4.58

Silica grafted with silanized carbon dots as a nano-on-micro packing material with enhanced hydrophilic selectivity

Cai Tianpei,Zhang Haijuan,Rahman A. F. M. Mustafizur,Shi Yan-Ping,Qiu Hongdeng

Carbon dots derivatized from N-(β-aminoethyl)-γ-aminopropyl-methyldimethoxysilane (AEAPMS) were coated onto silica microparticles. These particles (Sil-CDs) are shown to be an excellent stationary phase for use in hydrophilic interaction chromatography. Analytes including sulfonamides, nucleosides and bases, flavones and amino acids can be well separated on this stationary phase. Compared to a silica stationary phase functionalized with AEAPMS only, the Sil-CDs show enhanced separation performance. The selectivity factors of three nucleosides and bases (1.02–1.09) and four sulfonamides (1.04–1.11) on AEAPMS functionalized silica stationary phase were improved to 1.10–1.20 and 1.13–1.15 respectively on Sil-CDs stationary phase. This is attributed to the higher number of surface functional groups due to the introduction of carbon dots. The successful application of the Sil-CDs stationary phase highlights the potential of carbon dots as a modified material in chromatography. Schematic presentation of the preparation of silanized carbon dots coated onto silica microparticles. The material represents a new stationary phase for hydrophilic interaction chromatography. It shows improved separation performance compared to a silane-only functionalized silica stationary phase.

研究领域: 分析化学 · 材料科学
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JOURNAL OF MOLECULAR STRUCTURE · 2015 · IF 1.602

Mechanism of curcumin-induced trypsin inhibition: Computational and experimental studies

Yan-Qing Wang,Hong-Mei Zhang,Yi-Jun Kang,Yun-Lan Gu,Jian Cao

In the present study, the experimental and theoretical methods were used to analyze the binding interaction of food dye , curcumin with trypsin. The results of fluorescence spectroscopic measurements indicated that curcumin binding resulted in the obviously intrinsic fluorescence quenching with the increase concentration of curcumin. This binding interaction is a spontaneous process with the estimated enthalpy and entropy changes being −15.70 kJ mol −1 and 40.25 J mol −1  K −1 , respectively. Hydrogen bonds and hydrophobic forces played an important role in the complex formation between curcumin and trypsin. Moreover, curcumin could enter into the primary substrate-binding pocket and makes the activity of trypsin decrease remarkably with the increasing concentration of curcumin.

CAS / MDL: 458-37-7
研究领域: 生物化学 · 分子生物学 · 药物化学
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JOURNAL OF CHROMATOGRAPHY A · 2019 · IF 3.858

Polyethyleneimine-functionalized carbon dots and their precursor co-immobilized on silica for hydrophilic interaction chromatography

Tianpei Cai,Haijuan Zhang,Jia Chen,Zhan Li,Hongdeng Qiu

A new strategy based on synergistic effect of the carbon dots and their precursor was proposed to enhance the selectivity of hydrophilic interaction liquid chromatography (HILIC). In this work, polyethyleneimine (PEI) and PEI-functionalized carbon dots (PEICDs) mix-grafted silica packing material was prepared to act as a novel HILIC stationary phase. Both inner and outer surface of the porous silica are decorated with the mixture of PEI and carbon dots. This stationary phase, namely Sil-PEI/CDs, demonstrate enhanced retention ability and selectivity toward polar analytes, with which 11 nucleosides and nucleobases and 9 ginsenosides can be nicely separated. The Sil-PEI/CDs (RSD 0.12% – 0.54%) exhibited even better stability than the traditional PEI modified stationary phase (RSD 0.39% – 0.87%) within 40 h of continuously elution. And excellent column efficiency was observed from Sil-PEI/CDs (∼65,000 plates/m for cytidine). The strategy of mixed stabilization revealed a new method to prepare good performanced carbon dots based chromatographic column.

研究领域: 分析化学 · 材料科学
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FOOD HYDROCOLLOIDS · 2024 · IF 11

Advancing the pH-driven encapsulation technique of curcumin: Molecular interaction shifts due to structural and charge variations

Hanyu Li,Minghui Zhao,Jinghong Li,Jiaqi Wang,Huajiang Zhang,Jing Wang,Ning Xia,Zhongjiang Wang,Ahmed M. Rayan

The pH-driven method, recognized for its material safety and avoidance of organic solvents, is considered a promising approach for the encapsulation of hydrophobic active substances. However, the interaction mode and mechanism between carriers and receptors in two stages (alkalization and neutralization) remain underexplored. In this study, the hydrophilic globular protein ovalbumin (OVA) was utilized as a carrier to load curcumin (Cur) by the pH-driven method, with an alkalization pH of 8–12. The results indicated that the solubility of Cur and the degree of protein unfolding increased with increasing alkalization pH, with a transformation in the secondary structure observed at pH 12. During the alkalization stage at pH 11 and 12, the loading efficiency of Cur exceeded 90%, with binding constants reaching as high as 5.79 × 10 5  M −1 and 1.44 × 10 5  M −1 , respectively. The interactions transitioned through three phases in the alkalization process: electrostatic dominance to hydrophobic dominance, electrostatic assistance to hydrophobic dominance, and electrostatic repulsion hindrance. Notably, the generation of electrostatic repulsion and the potential loss of binding sites resulted in a decrease in the binding affinity between OVA and Cur at pH 12. In the neutralization stage, a stable structure dominated by hydrogen bonds and van der Waals forces was observed, with Cur encapsulated within the hydrophobic core of OVA. The mechanism proposed in this study elucidates the factors affecting the efficacy of the pH-driven method and helps to refine the application in hydrophobic active substance delivery systems.

研究领域: 食品科学 · 生物化学 · 药物递送系统
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MACROMOLECULAR RAPID COMMUNICATIONS · 2025 · IF 4.3

Xanthium-Inspired Microsphere Morphology Depends on the Dual Self-Assembly Behavior of Macromolecules

Luyao Xing,Jiaqiang Ding,Jiaqi Gao,Dongliang Chen,Chengdong Xiong,Zuochun Xiong

The self-assembly of macromolecular segments promotes the fabrication of polymer microspheres with multiple morphologies. Inspired by the xanthium shells, A dual-driven self-assembly method have defined that enables the construction of multi-dimensional morphologies on the microsphere surface at emulsion-confined interfaces. The two driving forces are derived from the phase separation caused by the immiscibility of macromolecular segments and the different interactions between chain segments of different hydrophilicity and water molecules. The synergistic effects of these two forces, the xanthium shell structure is constructed on the microsphere surface, enabling the development of increasingly complex superstructure. This scalable approach provides extensive potential for the self-assembly technology of block copolymers with opposite properties.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 高分子化学 · 仿生学
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JOURNAL OF CHROMATOGRAPHY A · 2025 · IF 4

Fabrication and evaluation of a dual-zwitterionic functionalized hydrophilic monolith for chromatographic separation

Liang Lai,Hongying Lan,Hui Huang,Tong Li,Kesara Ar-sanork,Jia-Huan Qu,Dongsheng Xu,Zhengjin Jiang

In this study, the chromatographic performance of a novel dual-zwitterionic hydrophilic stationary phase were investigated. Three zwitterionic HILIC monoliths were prepared using 3-(4-((methacryloyloxy)methyl)-1-methylpiperidin-1-ium-1-yl)propane-1-sulfonate (MAMMPS), 2-methacryloyloxyethyl phosphorylcholine (MPC), and a combination of MAMMPS and MPC (1:1, molar ratio) with N,N' -methylenebisacrylamide (MBA), separately. The monoliths exhibited good repeatability and stability. A high column efficiency of 120,000 plates/m was reached on the novel dual-zwitterionic functionalized poly(MAMMPS@MPC- co -MBA) monolith. Through the analysis and testing with different standards, the poly(MAMMPS@MPC- co -MBA) monolith exhibited the strongest retention capacity for negatively charged benzoic acid derivatives due to its high hydrophilicity and weak electronegativity. In contrast, the poly(MPC- co -MBA) monolith, functionalized with a single zwitterion, facilitated electrostatic interactions with negatively charged analytes. Baseline separation was achieved on all three monoliths for selected nucleobases, nucleosides, phenol derivatives, and amine compounds. However, their retention strength was mainly related to the hydrophilicity of the stationary phases, while hydrogen bonding and electrostatic interactions played secondary roles. Among the monoliths, the poly(MAMMPS- co -MBA) monolith demonstrated the best separation for neutral, acidic, and alkaline compounds. These findings offer valuable insights for the future selection and application of dual-zwitterionic HILIC monoliths for chromatographic separations.

研究领域: 分析化学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2015 · IF 2.858

Study on interaction between curcumin and pepsin by spectroscopic and docking methods

Ming Ying,Fengwen Huang,Haidong Ye,Hong Xu,Liangliang Shen,Tianwen Huan,Shitong Huang,Jiangfeng Xie,Shengli Tian,Zhangli Hu,Zhendan He,Jun Lu,Kai Zhou

The interaction between curcumin and pepsin was investigated by fluorescence, synchronous fluorescence, UV–vis absorption, circular dichroism (CD), and molecular docking. Under physiological pH value in stomach, the fluorescence of pepsin can be quenched effectively by curcumin via a combined quenching process. Binding constant ( K a ) and binding site number ( n ) of curcumin to pepsin were obtained. According to the theory of Förster's non-radiation energy transfer, the distance r between pepsin and curcumin was found to be 2.45   nm within the curcumin–pepsin complex, which implies that the energy transfer occurs between curcumin and pepsin, leading to the quenching of pepsin fluorescence. Fluorescence experiments also suggest that curcumin is located more closely to tryptophan residues than tyrosine residues. CD spectra together with UV–vis absorbance studies show that binding of curcumin to pepsin results in the extension of peptide strands of pepsin with loss of some β-sheet structures. Thermodynamic parameters calculated from the binding constants at different temperatures reveal that hydrophobic force plays a major role in stabilizing the curcumin–pepsin complex. In addition, docking results support the above experimental findings and suggest the possible hydrogen bonds of curcumin with Thr-77, Thr-218, and Glu-287 of pepsin, which help further stabilize the curcumin–pepsin complex.

CAS / MDL: 9001-75-6
研究领域: 生物化学 · 药物化学 · 分子生物学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2013 · IF 1.977

Comparative study of the binding of Trypsin with bifendate and analogs by spectrofluorimetry

Hua Li,Juanjuan Pu,Yi Wang,Chuang Liu,Jie Yu,Tao Li,Ruiqiang Wang

The interactions between Trypsin and bifendate (DDB) or analogs (I, II and III) were investigated by fluorescence, UV–visible absorption, resonance light scattering, synchronous fluorescence and 3D spectroscopy under mimic physiological conditions. The results revealed that DDB and analogs caused the fluorescence quenching of Trypsin by the formation of DDB/I/II/III–Trypsin complex. The quenching and energy transfer mechanisms were discussed. The binding constants and thermodynamic parameters at three different temperatures were obtained. The hydrophobic interaction was the predominant intermolecular forces to stabilize the complex. Results showed that DDB was the stronger quencher and bound to Trypsin with higher affinity than other three analogs.

CAS / MDL: 9002-07-7
研究领域: 生物化学 · 药物化学 · 分子生物学
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