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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

Surface-induced interaction of colloidal particles in isotropic liquid crystals

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Communications in Theoretical Physics 2024年第7期76卷 114-122页

作者： Hualing Zhang Kaifeng Weng Rui Ma Department of Physics College of Physical Science and TechnologyXiamen UniversityXiamen 361005China Fujian Provincial Key Laboratory for soft Functional Materials Research Research Institute for Biomimetics and Soft MatterXiamen UniversityXiamen 361005China

In this work,we study the interaction between two colloidal particles in a liquid crystal that is in the isotropic *** interaction is caused by surface-induced polarization of the liquid crystal molecules in the vicinity of the *** find that the interaction is short-ranged in both 2D and 3D *** symmetric homeotropic anchoring conditions,the interaction is *** under anti-symmetric homeotropic anchoring conditions,the interaction is repulsive at short distances but attractive at intermediate *** particle size has a strong impact on the effective interaction force.

关键词： surface-induced interaction colloidal particles liquid crystals

Structure regulating of metal clusters in carbonized metallic organic frameworks for high-efficient microwave absorption via tuning interaction strength between metals and ligands

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Nano Research 2024年第3期17卷 1699-1709页

作者： Chang Sun Kun-Yan Zhao Ming-Lu Huang Cheng-Long Luo Xu-Dong Chen Ming Wang School of chemistry and Chemical Engineering Chongqing Key Laboratory of Soft-Matter Material Chemistry and Function ManufacturingSouthwest UniversityChongqing 400715China Jieyang Branch of chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China

Carbonized metallic organic frameworks(CMOF)have been attracting attention in microwave absorption(MA)research area because of their diverse structures,tunable compositions,and rich ***,structure regulation on metal clusters in CMOF is achieved by tuning the interaction strength between metals and ligands to enhance microwave absorption *** to relatively weak interaction among copper cations and ligands,copper nanoclusters(CuNC)can be uniformly formed and embedded within the cobalt/zinc(Co/Zn)***,copper cations are added to the Co/Zn bimetallic zeolitic imidazolate frameworks(ZIFs).Secondly,the CMOF composite particles with CuNCs(CuNCs/CoZn-CMOF)were developed by a pyrolysis *** CuNCs/CoZn-CMOF with an appropriate amount of CuNCs can harmonize both dielectric and magnetic *** a result,the minimum reflection loss(RLmin)reaches–45.1 dB at a matching thickness of 2.30 mm and the effective absorption bandwidth(EAB)is 8.80 GHz at a thickness of 3.10 *** broadband response to electromagnetic waves is attributed to interfacial polarization at CuNCs surface and heterogeneous interfaces,impedance matching and multiple scattering of electromagnetic *** study provides a feasible method to develop CMOF microwave absorption materials with high EAB values.

关键词： heterogeneous interface carbonized metallic organic frameworks microwave absorption interfacial polarization

Highly selective adsorption of rhenium by amyloid-like protein material

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Science China(Technological Sciences) 2024年第5期67卷 1417-1430页

作者： MUHAMMAD Arif YANG QingMin KANWAL Aisha ZHAO Jian NAWAZ Mohsan REN Hao YANG Peng Key Laboratory of Applied Surface and Colloid chemistry Ministry of Education Xi’an Key Laboratory of Polymeric soft matter International Joint Research Center on Functional Fiber and Soft Smart TextileSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an710119China School of chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an710072China

Rhenium separation from molybdenum in molybdenite minerals and waste leachate has become an emerging *** this challenge,we prepared a set of protein-based alkylamine/alkylammonium salts complexes as extractants for selective uptake of rhenium from molybdenum,where the protein component turned into the insoluble amyloid-like structure when its internal disulfide bonds were reduced,namely phase-transition *** them,the phase-transited lysozyme and methyletrioctyleammonium chloride complex(PTL-N263)exhibited the most efficient adsorption at the alkaline condition for the electrostatic interaction between negatively charged metal ions with positively charged center(R_(4)N^(+))in N263,where negatively charged protein residues hindered the ion exchange of Cl^(-)in N263 for larger size Mo species(Mo_(7)O_(24)^(6-))than smaller size Re species(ReO^(4-)).The adsorption follows the Freundlich model and pseudo-second-order kinetics,which exhibits toplevel adsorption performance with a maximum adsorption capacity of 124 mg/g and a separation factor(β_(Re/Mo))of 2.78×10^(3)for *** adsorption capacity per unit area(57.2 mg/(g m^(2)))is 1.6–41 times higher than previously reported adsorbents,and the cost for adsorbing 1 g of Re(VII)is$1.07,indicating its industrial *** adsorption strategy can be applied to separating Re from Mo in binary solutions and industrial wastewater with other competing ions.

关键词： amyloid phase-transited lysozyme selective adsorption rhenium waste leachate solution

Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano Research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)*** herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) *** surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) *** example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V ***,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl *** virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and *** this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed *** work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

Tailoring the Properties of Polyhydroxyalkanoates from Plastics to Elastomers via Stereoselective Copolymerizations of rac-β-Butyrolactone and β-Propiolactone

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Chinese Journal of chemistry 2024年第9期42卷 963-972页

作者： Haoran Zhang JiaojiaoQin Xiaoyan Tang Beijing National Laboratoryfor Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCenterfor Soft Matter Science and EngineeringCollegeof Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Poly(3-hydroxybutyrate),a crucial member of the large biodegradable polyhydroxyalkanoate family,suffers from its *** enhance its performance,we employed a straightforward approach involving the ring-opening copolymerization of racemic-β-butyrolactone(rac-β-BL)andβ-propiolactone(β-PL)using the syndio-selective amino-alkoxy-bis(phenolate)-yttrium complex as a catalyst,thanks to the excellent ductility of poly(3-hydroxypropionate).Control over the rac-β-BL/β-PL feeding ratios and polymerization time yielded random or block copolymers with tunable thermal and mechanical properties comparable to traditional fossil-based ***,we achieved one-pot synthesis of hard-soft-hard triblock copolymers by exploiting monomers’different copolymerization rates and a bifunctional initiator,thus transforming polyhydroxyalkanoates from hard and tough plastics to soft and ductile thermoplastic elastomers.

关键词： Ring-opening(co-)polymerization Biodegradable polymers Polyhydroxyalkanoates Copolymers Plastics Elastomers

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

Unlocking the Potential of Poly(butylene succinate)through Incorporation of Vitrimeric Network Based on Dynamic Imine Bonds

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Chinese Journal of Polymer Science 2024年第10期42卷 1414-1424,I0006页

作者： Shan-Song Wu Hui-Juan Lu Yi-Dong Li Shui-Dong Zhang Jian-Bing Zeng Chongqing Key Laboratory of soft-matter Material Manufacturing School of Chemistry and Chemical EngineeringSouthwest UniversityChongqing400715China School of Mechanical and Automotive Engineering South China University of TechnologyGuangzhou510640China

Poly(butylene succinate)(PBS)exhibits many advantages,such as renewability,biodegradability,and impressive thermal and mechanical properties,but is limited by the low melt viscosity and strength resulted from the linear *** address this,vitrimeric network was introduced to synthesize PBS vitrimers(PBSVs)based on dynamic imine bonds through melt polymerization of hydroxyl-terminated PBS with vanillin derived imine containing compound and hexamethylene diisocyanate using trimethylolpropane as a crosslinking *** with different crosslinking degrees were synthesized through changing the content of the crosslinking *** effect of crosslinking degree on the thermal,theological,mechanical properties,and stress relaxation behavior of the PBSVs was studied in *** results demonstrated that the melt viscosity,melt strength,and heat resistance were enhanced substantially without obvious depression in crystallizability,thermal stability,and mechanical properties through increasing crosslinking *** addition,the PBSVs exhibit thermal reprocessability with mechanical properties recovered by more than 90%even after processing for three ***,PBSV with improved melt properties shows significantly improved foamability compared to commercial *** research contributes to the advancement of polymer technology by successfully developing PBS vitrimers with improved properties,showcasing their potential applications in sustainable and biodegradable materials.

关键词： Poly(butylene succinate) Vitrimer Imine bonds Foamability

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