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Dual-functional poly(2-methyl-2-oxazoline)/poly(2-(dimethylamine)ethyl methacrylate)mixed brushes with switchable protein adsorption and antibacterial properties

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Chinese Journal of Chemical Engineering 2024年第2期66卷 19-30页

作者： Kang He Liangyu Zhu Yanmei Wang cas key laboratory of soft matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Herein,binary mixed brushes consisting of poly(2-methyl-2-oxazoline)(PMOXA)and poly(2-(dimethylamine)ethyl methacrylate)(PDMAEMA)with different chain lengths were fabricated by successive grafting of NH_(2)-terminated PMOXA and SH-terminated PDMAEMA onto polydopamine-anchored *** mixed-brush coating was characterized by variable-angle spectroscopic ellipsometry,X-ray photoelectron spectroscopy,Fourier transform infrared spectroscopy,zeta potential measurements,water contact angle,and atomic force *** mixed brushes showed tunable surface charge,wettability,and surface roughness,depending on the degree of PDMAEMA swelling under varying pH and ionic strength(Ⅰ).Then the adsorption behaviors of pepsin,bovine serum albumin(BSA),γ-globulin,and lysozyme,four very different proteins with regard to isoelectric point,on the mixed brushes coating were studied by using fluorescence microscopy and surface plasmon *** the chain length of PDMAEMA was about twice as long as PMOXA,the mixed brushes not only had high adsorption capacity for pepsin,BSA,and y-globulin but also had a desorption efficiency of 86.9%,87.1%,and 93.5%,*** is explained that electrostatic attraction between the protonated PDMAEMA and positively charged acidic proteins(pepsin and BSA,whose isoelectric points were below the pK_(a) of PDMAEMA)would drive the intensive adsorption(at pH 3,I=10^(-3)mol·L^(-1)for pepsin,and pH 5,I=10^(-5)mol·L^(-1)for BSA),while desorption was dominated by the hydrophilic PMOXA when PDMAEMA was shrinking(at pH 7,I=10^(-1)mol·L^(-1)for pepsin,and pH 9,I=10^(-1)mol·L^(-1)for BSA).Furthermore,the isoelectric precipitation led to the adsorption of neutral protein(γ-globulin,whose isoelectric point was near the pK_a of PDMAEMA)at pH 7,I=10^(-5)mol·L^(-1),while electrostatic repulsion and antifouling PMOXA triggered the desorption of y-globulin at pH 3,I-10^(-1)mol·L^(-1).However,alkaline protein(lysozyme,whose isoelectric point was higher than

关键词： Switchable conformation transition Controllable protein adsorption Mixed brushes Isoelectric point Antibacterial surface

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Chain Dynamics Heterogeneity in Plasticized Poly(vinyl butyral)(PVB) as Elucidated by Solid-State NMR

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Chinese Journal of Polymer Science 2024年第1期42卷 113-124,I0010页

作者： Jing Lv Xu Chen Zi-Shuo Wu Ya-Hui Li Wei Chen National Synchrotron Radiation laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer FilmCAS Key Laboratory of Soft Matter ChemistryUniversity of Scienceand Technology of ChinaHefei 230026China

The chain dynamics heterogeneity of the poly(vinyl butyral)(PVB) plasticized by triethylene glycol bis(2-ethylhexa noate)(TEG-EH) was investigated by various solid-state NMR *** plasticized PVB shows two domains in distinct molecular dynamics differences,namely,rigid and soft domains,where the latter is the plasticizer-rich *** time domain low field NMR was first used to investigate the dynamics heterogeneity of the plasticized PVB,and the results show the decreasing activated energy of components in the soft domain of plasticized PVB(E_a=20.2 kJ/mol) as compared with that of the pristine one(E_a=24.3 kJ/mol).Detailed dynamics heterogeneity was obtained by high-field NMR with site-specific *** quadrupole-echo ~2H-NMR was adopted to elucidate the dynamics heterogeneity of the vinyl alcohol(VA) units,where only the hydroxyl group of VA is *** ~1H-^(13)C WISE NMR spectra show that there is not much difference in the mobility of the VB unit in PVB with and without plasticizer,whereas the glass transition temperature differed by approximately 53℃.This is further supported by Torchia's T_1 relaxation *** origin of such an unusual phenomenon is attributed to the critical role of the remaining VA(~22%) in the soft domain,where the VA units locally aggregate through hydrogen ***,the existence of a mobility gradient in the VB unit has been ***,the mobility difference for VB with different stereo-geometry(meso or racemic conformation) is observed for the first *** indicates the importance of modulating the ratio of meso over racemic VB for controlling the macroscopic perfo rmance of PVB.

关键词： Poly(vinyl butyral) Dynamics heterogeneity Plasticizer Solid state NMR

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Double stimulus-responsive palladium catalysts for ethylene polymerization and copolymerization

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Chinese Chemical Letters 2024年第7期35卷 407-411页

作者： Hailong He Wenbing Wang Wenmin Pang Chen Zou Dan Peng cas key laboratory of soft matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei National Laboratory for Physical Sciences at the MicroscaleHefei 230026China

The external stimulus response strategy has been evolved rapidly in the field of olefin *** this work,we modularly synthesized three types of double stimulus responsiveα-diimine palladium catalysts,combining redox regulation and other regulation together,such as light,Lewis acid and alkali *** catalytic activities and the molecular weight of polyethylene products can be regulated for 4 times in ethylene *** palladium complexes were also used for the copolymerization reaction of ethylene and polar monomers,such as methyl 10-undecylenate and methyl acrylate,effectively regulating the catalytic activities,the molecular weight and polar monomer incorporation of the prepared *** research on these dual-regulated palladium complexes makes full use of prepared catalysts and provides new inspirations for regulating olefin polymerization.

关键词： Dual-regulated Stimulus-responsive Palladium Ethylene polymerization Polar monomer

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Polyolefin vitrimers bearing acetoacetate functionality

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Science China Chemistry 2024年第11期67卷 3861-3867页

作者： Zihao Wang Yue Liu Wenmin Pang Ao Chen Min Chen Chinese Academy of Sciences (cas) key laboratory of soft matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Anhui University

Polyolefin vitrimers are polymer networks bearing reversible covalent crosslinking points, enabling them to be reprocessed and recycled. In this contribution, a series of polyolefin vitrimers were designed based on the acetoacetate-functionalized polyolefin copolymers, which were produced through the direct copolymerization of ethylene with polar comonomers using a phosphinesulfonate palladium catalyst. The pendant acetoacetate group could mediate several characteristic reactions, such as the Michael addition reaction, ketone-amine condensation and metal coordination reaction. As such, structurally adjustable polyolefin vitrimers can be accessed by introducing various dynamic crosslinking bonds, including disulfide exchange, transamination of vinylogous urethane and labile metal coordination bond. The utilization of different crosslinking reactions and the mole ratio of crosslinkers significantly impact the material properties of the resultant polymers. Specifically, the generated polyolefin vitrimers demonstrated excellent reprocessability and closed-loop recycling properties. The study in this work provides an efficient strategy to access various polyolefin vitrimers.

关键词： polyolefin vitrimers acetoacetate group polar monomer olefin copolymerization

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Competition of Composition Fluctuation Modes in Weakly Segregated Salt-doped Symmetric Diblock Copolymers

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Chinese Journal of Polymer Science 2024年第9期42卷 1375-1385,I0008页

作者： Yuan-Xin Zhou Xian Kong South China Advanced Institute for soft matter Science and Technology School of Emergent Soft MatterSouth China University of TechnologyGuangzhou510640China Guangdong Provincial key laboratory of Functional and Intelligent Hybrid Materials and Devices South China University of TechnologyGuangzhou510640China

Salt-doped block copolymers have widespread applications in batteries,fuel cells,semiconductors,and various industries,where their properties crucially depend on phase separation ***,investigations into salt-doped diblock copolymers have predominantly focused on microphase separation,overlooking the segregation between ionic and polymeric *** study employs weak segregation theory to explore the interplay between phase separation dominated by the polymer-modulated mode and the salt-out-modulated mode,corresponding to microscopic and macroscopic phase separations,*** comparing diblock copolymers doped with salts to those doped with neutral solvents,we elucidate the significant role of charged species in modulating phase *** phase separation mode exhibits a transition between the polymer-modulated and salt-out-modulated modes at different *** systems doped with neutral solvents,this transition is stepwise,while in salt-ion-doped systems,it is *** a sufficiently large Flory-Huggins parameter between ions and polymers,the salt-out-modulated mode becomes dominant,promoting macrophase *** to the solvation effect of salt ions,salt-doped systems are more inclined to undergo microphase ***,we explore factors influencing the critical wavenumber of phase separation,including doping level and the Flory-Huggins parameters between two blocks and between ions and polymeric *** findings reveal that in a neutral solvent environment,these factors alter only the boundary between micro-and macro-phase separations,leaving the critical wavenumber unchanged in microphase separation ***,in a salt-doped environment,the critical wavenumber of microphase separation varies with these *** provides valuable insights into the pivotal role of electrostatics in the phase separation of salt-doped block copolymers.

关键词： Block copolymer Phase separation Field theory Salt-doped

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Highly elastic and degradable vitrimeric elastomers using polycondensation

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Chinese Chemical Letters 2024年第3期35卷 434-438页

作者： Yue Liu Yongshuang Huang Chao Li Guifu Si Min Chen Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China cas key laboratory of soft matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Introducing covalently crosslinked network to polymer matrix can merge the advantages in reprocessing and durability of *** this contribution,a series of high-performance vitrimeric elastomers were achieved via *** topological structures of polymers were tuned by varying the feeding ratios of bisacetoacetate,hex–substituted bisacetoacetate,bisamine and tris(2-aminoethyl)*** these structural manipulations,the vitrimeric elastomers presented great elastic recovery properties(strain recovery value up to 80%)benefiting from the introduction of long chain ***,the elastomers exhibited excellent reprocessing property,water vapor/oxygen barrier and adhesive ***,the elastomers could be degraded into monomer under acid conditions which enabled the elastomer synthesis again in closed loop recycling *** ease of the polycondensation in this work to prepare highly elastic and recyclable vitrimeric elastomers demonstrated exciting opportunities for the synthesis of sustainable polymers.

关键词： Polycondensation Vitrimeric elastomers Highly elastic Degradable polymers

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3D Foam-Based MXene Architectures:Structural and Electrolytic Engineering for Advanced Potassium-Ion Storage

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Energy & Environmental Materials 2024年第4期7卷 64-73页

作者： Peng Zhang Yanmeng Peng Qizhen Zhu Razium Ali Soomro Ning Sun Bin Xu State key laboratory of Organic-Inorganic Composites Beijing Key Laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical Technology Beijing Advanced Innovation Centre for soft matter Science and Engineering Beijing University of Chemical Technology

MXenes are emerging rapidly as promising electrode materials for energy storage due to their high electronic conductivity and rich surface chemistry,but their potassium storage performance is unsatisfactory because of... 详细信息

关键词： 3D foam-like scaffold electrolyte chemistry electrostatic neutralization MXene potassium-ion batteries

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Novel photoresponsive dinuclear nickel catalysts for ethylene(co)polymerization

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Science China Chemistry 2024年

作者： Chenlong Nan Tong Pang Jiaxing Zhao Lijia Fan Chen Zou Xin-Qi Hao Mao-Ping Song Jun-Fang Gong Changle Chen Hui Jiang College of Chemistry Pingyuan Laboratory Zhengzhou University cas key laboratory of soft matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China

Compared with the conventional strategies of electronic and/or steric perturbation, catalytic olefin polymerization modulated by light irradiation or metal-metal cooperativity effect is a fascinating challenge that attracts considerable attention in the academic community. In this context, we design a strategy that could employ both effects to influence the polymerization process. Some dinuclear salicylaldimine and α-imino-ketone nickel complexes bearing a stiff-stilbene bridge were prepared, which could transfer between(E)-isomers and(Z)-isomers under ultraviolet irradiation. This isomerization can tune the electronic, steric and metal-metal cooperativity effects of the nickel catalysts. In this way, the catalytic activity, as well as polymer microstructures including molecular weight and branching density can be modulated in ethylene polymerization and copolymerization *** strategy is generally applicable to other olefin polymerization catalytic systems and other types of transition metal mediated catalysis.

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Fine-tuning growth in gold nanostructures from achiral 2D to chiral 3D geometries

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Nano Research 2024年第7期17卷 6654-6660页

作者： Lili Tan Zhi Chen Chengyu Xiao Zhiyong Geng Yinran Jin Chaoyang Wei Fei Teng Wenlong Fu Peng-peng Wang State key laboratory for Mechanical Behavior of Materials Shaanxi International Research Center for Soft MatterSchool of Materials Science and EngineeringXi’an Jiaotong UniversityXi’an 710049China

Enriching the library of chiral plasmonic structures is of significant importance in advancing their applicability across diverse domains such as biosensing,nanophotonics,and ***,employing triangle nanoplates as growth seeds,we synthesized a novel class of chiral-shaped plasmonic nanostructures through a wet chemical strategy with dipeptide as chiral inducers,including chiral tri-blade boomerangs,concave rhombic dodecahedrons,and *** structural diversity in chiral plasmonic nanostructures was elucidated through their continuous morphological evolution from two-dimensional to threedimensional *** fine-tuning of chiroptical properties was achieved by precisely manipulating crucial synthetic parameters such as the amount of chiral molecules,seeds,and gold precursor that significantly influenced chiral structure *** findings provide a promising avenue for enriching chiral materials with highly sophisticated structures,facilitating a fundamental understanding of the relationship between structural nuances and chiroptical properties.

关键词： plasmonic nanostructures geometric chirality circular dichroism fine-tuning

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Sub-nanosized vanadate hybrid clusters maintain glucose homeostasis and restore treatment response in inflammatory disease in obese mice

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Nano Research 2024年第3期17卷 1818-1826页

作者： Kun Chen Shengqiu Liu Yujun Wei South China Advanced Institute for soft matter Science and Technology School of Emergent Soft MatterSouth China University of TechnologyGuangzhou 510641China Guangdong Provincial key laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing South China University of TechnologyGuangzhou 510641China Guangdong Provincial key laboratory of Functional and Intelligent Hybrid Materials and Devices South China University of TechnologyGuangzhou 510641China

Obesity is closely related with insulin resistance and chronic ***,we report that unsaturated lipid-modified polyoxovanadates(ULPOVs)can restrict weight gain of diet-induced obese mice and improve their glycemic control and obesity-associated *** administration of the sub-nanosized ULPOVs at a low dosage for 7 weeks reduces the body weight and almost normalizes the blood glucose levels of obese mice fed on a high-fat *** treatment increases the activity of the nuclear receptor peroxisome proliferator-activated receptorγ(PPARγ)and reduces intestinal caloric intake,which may be the main reason for blood sugar and body weight *** addition to insulin-sensitizing,PPARγactivation induced by ULPOV treatment in obese mice with atopic dermatitis(AD)promotes the type 2 T helper(TH_(2))cell selective responses and therapeutic effects on immune dysregulation caused by *** data suggest sub-nanosized polyoxovanadate clusters as a class of potential candidates to relieve symptoms accompanied by diet-induced obesity.

关键词： polyoxovanadates lipid modification glucose homeostasis obesity inflammatory disease peroxisome proliferator-activated receptorγ(PPARγ)

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