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Polyelectrolyte Complexes and Coacervates Formed by De novo-Designed Peptides and Oligonucleotide

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Chinese Journal of polymer Science 2024年第9期42卷 1333-1340,I0007页

作者： Tian-Hao Ren De-Hai Liang Beijing National Laboratory for Molecular Sciences Department of Polymer Science and Engineering and the Key Laboratory of Polymer Chemistry and Physics of the Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

The liquid-liquid phase separation of biopolymers in living cells contains multiple interactions and occurs in a dynamic *** the regulation mechanism is still a *** this work,we designed a series of peptides(XXLY)_(6)SSSGSS and studied their complexation and coacervation behavior with single-stranded ***“X”and“Y”are varied to combine known amounts of charged and non-charged amino acids,together with the introduction of secondary structures and pH *** show that the electrostatic interaction,which is described as charge density,controls both the strength of complexation and the degree of chain relaxation,and thus determines the growth and size of the *** hydrophobic interaction is prominent when the charges are ***,the secondary structures of peptides exhibit profound effect on the morphology of the phases,such as solid phase to liquid phase *** study gains insight into the phase separation under physiological *** is also helpful to create coacervates with desirable structures and functions.

关键词： Polyelectrolyte complex Coacervate Peptides Secondary structure Electrostatic interaction

Cross-linked Electrospun Gel polymer Electrolytes for Lithium-Ion Batteries

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Chinese Journal of polymer Science 2024年第8期42卷 1021-1028页

作者： Xue Gong Qin Xiao Qing-Yin Li Wen-Cui Liang Feng Chen Long-Yu Li Shi-Jie Ren College of polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China

Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage ***,a series of precursor membranes with high porosity were produced using electrospinning technology by mixing PVDF and triblock copolymer(PS-PEO-PS),resulting in a porous structure with good interconnections,which facilitates the absorbency of a large amount of electrolyte and further increases the ionic conductivity of gel polymer electrolytes(GPEs).It has been demonstrated that post-cross-linking of the precursor membranes increa ses the rigidity of the nanofibers,which allows the polymer film to be dimensionally sta ble up to 260℃while maintaining superior electrochemical *** obtained cross-linked GPEs(CGPEs)showed high ionic conductivity up to 4.53×10^(-3)S·cm^(-1).With the CGPE-25,the assembled Li/LiFeP04 half cells exhibited good rate capability and maintained a capacity of 99.4%and a coulombic efficiency of99.3%at 0.1 *** results suggest that the combination of electrospinning technique and post-cross-linking is an effective method to construct polymer electrolytes with high thermal stability and steadily decent electrochemical performance,particularly useful for Lithium-ion battery applications that require high-temperature usage.

关键词： Electrospinning Cross-linked Gel polymer electrolytes Lithium-ion batteries

An Effective Approach for the Preparation of High Performance Thermal Conductive polymer Composites Containing Liquid Metal

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Chinese Journal of polymer Science 2024年第7期42卷 992-1001,I0010页

作者： Xin Chen Xue-Zhong Zhang Yi-Fei Yuan Chuan-Liang Chen Lian-Hu Xiong Qiang Fu Hua Deng College of polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065China department of Materials Science and Engineering Sichuan University-Pittsburgh InstituteSichuan UniversityChengdu610065China

The preparation of high-performance thermal conductive composites containing liquid metals(LM)has attracted significant ***,the stable dispersion of LM within polymer solution and effective property contribution of liquid metals remains significant challenges that need to be *** by the properties of the dendritic structure of the tree root system in grasping the soil,“shear-induced precipitation-interfacial reset-reprotonation”processing strategy is proposed to prepare nanocomposites based on aramid micron fibers(AMFs)with hierarchical dendritic *** to the combination of van der Waals force provided by hierarchical dendritic structure,electrostatic interaction between AMFs and LM,coordinative bonding of―NH to LM,together with interfacial re-setting and multi-step protonation,several features can be achieved through such strategy:conducive to the local filler network construction,improvement of interfacial interaction,improvement of the stability of filler dispersion in the solvent,and enhancement of mechanical and thermal properties of the *** resulting AMFsp H=4/LM films demonstrate a thermal conductivity of 10.98 W·m^(-1)·K^(-1)at 70%filler content,improvement of 126.8%compared to ANFs/LM film;while maintaining a strength of~85.88 MPa,improvement of 77%compared to AMFs/LM *** also possess insulation properties,enable heat dissipation for high power *** work provides an effective strategy for the preparation of high performance polymer composites containing liquid metal.

关键词： Shear-induced Reprotonation AMFs LM Filler dispersion

Shear-thinning Catechol-modified Chitosan Hydrogel Loaded with Silver Nanoparticles for Endoscopic Submucosal Dissection

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Chinese Journal of polymer Science 2024年第8期42卷 1147-1155页

作者： Wen-Jun Feng Yan-He Wu Xiao-Yang Liu Zheng-Ke Wang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310058China

Shear-thinning hydrogels have emerged for endoscopic submucosal dissection,while wound intervention after surgery has rarely been ***,a catechol-modified chitosa n hydrogel with shear-thinning property was developed for simultaneously facilitating endoscopic submucosal dissection and postoperative wound *** from the shear-thinning and self-healing characteristics,the asprepared hydrogel showed easily endoscopic *** also performed very well as submucosal cushion,which could remain above 70%after injection for 120 min in ex vivo porcine large intestine *** fact,the cushion height of normal saline dramatically decreased to 46%of the initial height at 30 *** nanoparticles encapsulated into the network endowed the hydrogel with almost reached 100%antibacterial effect against *** and *** hemolysis ratio of the hydrogel was calculated to be as low as 0.8%.Combined with good hemocompatibility and cytocompatibility,the as-prepared hydrogel displayed much higher in vivo wound closu re and healing efficacy than normal *** results demonstrated the superiority of the shear-thinning chitosan hydrogel in facilitating clinical endoscopic submucosal dissection surgery.

关键词： Shear-thinning hydrogel Endoscopic mucosal dissection Wound healing Catechol-modified chitosan Silver nanoparticles

Photoswitchable Spiropyridine Enabled Photoactuation of polymeric Hydrogels under Physiological pH Conditions

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Chinese Journal of polymer Science 2024年第10期42卷 1602-1609,I0015页

作者： Cong Liao Meng-Qi Du Chuang Li Key Laboratory of Precision and Intelligent Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaAnhui230026China

The incorporation of molecular switches into polymer networks has been a powerful approach for the development of functional polymer materials that display macroscopic actuation and function enabled directly by molecular ***,such materials sometimes require harsh conditions to perform their functions,and the design of new molecular photoswitches that can function under physiological conditions is highly ***,we report the design and synthesis of a spiropyridine-based photoswitchable hydrogel that exhibits light-driven actuation at physiological *** to its high p Ka,spiropyridine maintains its ring-open protonated form at neutral pH,and the resulting hydrogel remains in a swollen *** irradiation with visible light,the ring closure of spiropyridine leads to a decrease in the charge and a reduction in the volume of the *** contracted gel could spontaneously recover to its expanding state in the dark,and this process is highly dynamic and reversible when the light is switched on and ***,the hydrogel shows switchable fluorescence in response to visible *** deformation is observed in the hydrogel thin films upon irradiation from one ***,the independence of this spiropyridine hydrogel from the acidic environment makes it biotolerant and shows excellent *** biocompatible spiropyridine hydrogel might have important biorelated applications in the future.

关键词： Spiropyridine photowitch polymer hydrogel Photoactuation Physiological pH Biocompatibility

A Self-Healing Elastomer with Extremely High Toughness Achieved by Acylsemicarbazide Hydrogen Bonding and Cu^(2+)-Neocuproine Coordination Interactions

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Chinese Journal of polymer Science 2024年第10期42卷 1425-1434,I0007页

作者： Xiao-Ming An Yi-Ping Wang Tang-Song Zhu Chong Xing Xu-Dong Jia Qiu-Hong Zhang Key Laboratory of High Performance polymer Material and Technology of MOE Department of Polymer Science and EngineeringSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210093China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing210093China

Elastomers with high mechanical toughness can guarantee their durability during service ***-healing ability,as well as recyclability,can also extend the life of materials and save the consuming cost of the *** efforts have been dedicated to promoting the mechanical toughness as well as the self-healing capability of elastomers at the same time,while it remains a challenge to balance the trade-off between the above properties in one *** we proposed a molecular design driven by dual interactions of acylsemicarbazide hydrogen bonding and Cu^(2+)-neocuproine coordination *** introducing the reversible multiple hydrogen bonds and strong coordination bonds,we successfully fabricated an extremely tough and self-healing *** elastomer can achieve an impressive top-notch toughness of 491 MJ/m^(3).Furthermore,it boasted rapid elastic restorability within 10 min and outstanding crack tolerance with high fracture energy(152.6kJ/m^(2)).Benefiting from the combination of dynamic interactions,the material was able to self-repair under 80℃conveniently and could be reprocessed to restore the exceptional mechanical properties.

关键词： Metal-ligand coordination Hydrogen bond Ultra-tough elastomer Self-healing

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

Near-infrared non-fused electron acceptors for efficient organic photovoltaics

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Chinese Chemical Letters 2024年第4期35卷 436-441页

作者： Wenxiang Ma Xinyu He Tianyi Chen De-Li Ma Hongzheng Chen Chang-Zhi Li State Key Laboratory of Silicon and Advanced Semiconductor Materials Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

Developing narrow-bandgap organic semiconductors is important to facilitate the advancement of organic photovoltaics(OPVs). Herein, two near-infrared non-fused ring acceptors(NIR NFRAs), PTBFTT-F and PTBFTT-Cl have been developed with A-π_A-π_D-D-π_D-π_A-A non-fused structures. It is revealed that the introduction of electron deficient π-bridge(π_A) and multiple intramolecular noncovalent interactions effectively retained the structural planarity and intramolecular charge transfer of NFRAs, extending strong NIR photon absorption up to 950 nm. Further, the chlorinated acceptor, with the enlarged π-surface compared to the fluorinated counterpart, promoted not only molecular stacking in solid, but also the desirable photochemical stability in ambient, which are helpful to thereby improve the exciton and charge dynamics for the corresponding OPVs. Overall, this work provides valuable insights into the design of NIR organic semiconductors.

关键词： Organic photovoltaic Near-infrared Non-fused electron acceptor Noncovalent interaction Stability

Regulating photothermal properties of near-infrared croconaine dyes by supramolecular assembly

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Nano Research 2024年第9期17卷 8560-8570页

作者： Yangge Ren Yue Lu Juanjuan Gao Yi Ding Bo Zhu Xinyu Hou Lin Jia department of polymer Materials School of Materials Science and EngineeringShanghai UniversityShanghai 200444China department of Electronic Information Materials School of Materials Science and EngineeringShanghai UniversityShanghai 200444China

The photochemical and photophysical properties of near-infrared(NIR)dyes are significantly influenced by their aggregation state and mesoscopic ***,beyond chemical synthesis,the regulation mechanisms for the properties of NIR dyes,particularly with respect to photothermal properties of the aggregates,are not yet fully ***,we investigate the photothermal behaviors of croconaine-based(CroA)NIR dyes containing dipeptide or amino acids *** introduction of hydrogen bonding promotesπ-πstacking of croconaine center,which can efficiently regulate aggregation states and assembly structures in *** laser irradiation,CroA aggregates undergo aggregation-dissociation transition,the in-situ monomer generation process regulates two parameters of photothermal performance:heating rates and plateau photothermal *** study reveals the regulation effect of non-covalent bonding interactions on CroA aggregates,highlighting supramolecular assembly strategy not only facilitates to construct of photothermal nanomaterials with well-defined structures,but also provides an alternative and effective method for regulating photothermal performance of NIR dyes.

关键词： croconaine dye hydrogen bonding photothermal performance supramolecular assembly chirality