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Energy & Environmental Materials 2024年第2期7卷 200-208页

作者： Jiale Ke Xing Zhao Jie Yang Kai Ke Yu Wang Mingbo Yang Wei Yang College of Polymer Science and engineering Sichuan UniversityState Key Laboratory of Polymer Materials EngineeringChengdu 610065China

Thermoelectric(TE)generators capable of converting thermal energy into applicable electricity have gained great popularity among emerging energy conversion ***-based ionic thermoelectric(i-TE)materials are promising candidates for energy conversion systems because of their wide sources,innocuity,and low manufacturing ***,common physically crosslinked biopolymer gels induced by single hydrogen bonding or hydrophobic interaction suffer from low differential thermal voltage and poor thermodynamic ***,we develop a novel i-TE gel with supramolecular structures through multiple noncovalent interactions between ionic liquids(ILs)and gelatin molecular *** thermopower and thermoelectric power factor of the ionic gels are as high as 2.83 mV K-1 and 18.33μW m^(-1)K^(-2),*** quasi-solid-state gelatin-[EMIM]DCA i-TE cells achieve ultrahigh 2 h output energy density(E_(2h)=9.9 mJ m^(-2))under an optimal temperature ***,the remarkable stability of the supramolecular structure provides the i-TE hydrogels with a thermal stability of up to 80℃.It breaks the limitation that biopolymer-based i-TE gels can only be applied in the low temperature range and enables biopolymer-based i-TE materials to pursue better performance in a higher temperature range.

关键词： biopolymer gel ionic liquid multiple noncovalent interactions supramolecular structure thermoelectric conversion

In situ thermoresponsive supramolecular assembly for switchable circularly polarized luminescence

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Science China Chemistry 2024年第7期67卷 2362-2372页

作者： Menghan Pan Gong Zhang Haotian Ma Xiaoxiao Cheng Jieai Li Wei Zhang State and Local Joint engineering laboratory for Novel Functional Polymeric Materials Jiangsu Engineering Laboratory of Novel Functional Polymeric MaterialsSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China School of Chemical and Environmental engineering Anhui Polytechnic UniversityWuhu 241000China

The dynamic regulation of circularly polarized luminescence(CPL)holds profound significance in various fields,such as highlevel information storage and *** we developed a chiral amphiphilic molecule,CPSB-GLU-PEG350(CGP),composed of aggregation-induced emission(AIE)chromophores(Z)-4-(1-cyano-2-phenylvinyl)benzoic acid(CPSB),a chiral linker Glutamic acid and polyethylene glycol(PEG)thermoresponsive *** the self-assembled supramolecular system formed by CGP,we have achieved in-situ temperature-responsive chiral structures,facilitating the thermal control switch of the CPL *** dynamics simulations demonstrate the distinct behaviors of AIE and PEG units during the temperature-variable assembly ***,by co-assembling achiral dye molecules with CGP,we have expanded the color range of the temperature-responsive CPL assembly system in situ and confirmed the occurrence of circularly polarizedF?rster resonance energy transfer(C-FRET)phenomenon in this process,which successfully enriched the strategies for in-situ CPL control in aqueous *** addition,the contactless radiative energy transfer of CPL can also be realized in this system,exhibiting more flexible temperature regulation of the CPL *** study provides a convenient and universal strategy for the construction of dynamically smart chiroptical materials.

关键词： circularly polarized luminescence in-situ thermoresponsive supramolecular assembly energy transfer

Exploring Trade-offs in Thermal Interface Materials:The Impact of Polymer-Filler Interfaces on Thermal Conductivity and Thixotropy

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Chinese Journal of Polymer Science 2024年第7期42卷 916-925,I0006页

作者： Bin Zhang Zheng-Li Dou Yong-Zheng Zhang Qiang Fu Kai Wu College of Polymer Science and engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065China

Effective thermal transport across solid-solid interfaces which is essential in thermal interface materials(TIMs),necessitates both optimal thixotropy and high thermal *** role of filler surface modification,a fundamental aspect of TIM fabrication,in the influence of these properties is not fully *** study employs the use of a silane coupling agent(SCA)to modify alumina,integrating experimental approaches with molecular dynamics simulations,to elucidate the interface effects on thixotropy and thermal conductivity in polydimethylsiloxane(PDMS)-based *** findings reveal that the variations of SCAs modify both interface binding energy and transition layer *** interface binding energy restricts macromolecular segmental relaxation near the interface,hindering desirable thixotropy and bond line *** the contrary,the thickness of the transition layer at the interface positively influences thermal conductivity,facilitating the transport of phonons between the polymer and ***,selecting an optimal SCA allows a balance between traditionally conflicting goals of high thermal conductivity and minimal bond line thickness,achieving an impressively low interface thermal resistance of just 2.45-4.29 K·mm^(2)·W^(-1)at275.8 kPa.

关键词： Thermal interface material Surface modification Thermal conductivity Thixotropy Interface thermal resistance

Tough Semi-interpenetrating Polyvinylpyrrolidone/Polyacrylamide Hydrogels Enabled by Bioinspired Hydrogen-bonding Induced Phase Separation

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Chinese Journal of Polymer Science 2024年第5期42卷 591-603,I0006页

作者： Qiong-Jun Xu Zhao-Yang Yuan Chang-Cheng Wang Hao Liang Yu Shi Hai-Tao Wu Hu Xu Jing Zheng Jin-Rong Wu State Key laboratory of Polymer Materials engineering College of Polymer Science and EngineeringSichuan UniversityChengdu610065China

Semi-interpenetrating(semi-IPN)hydrogels formed by the continuous interpenetration of cross-linked polymer network and linear non-crosslinked polymer with multifunctionality are widely used in biomedical and other ***,the negative impact of linear polymer on the homogeneity of the cross-linked network often leads to a decrease in the mechanical properties of semi-IPN hydrogels and severely limits their ***,a bioinspired hydrogen-bonding induced phase separation strategy is presented to construct the tough semi-IPN polyvinylpyrrolidone/polyacrylamide hydrogels(named PVP/PAM hydrogels),including the linear polymer polyvinylpyrrolidone(PVP)and cross-linked polyacrylamide(PAM)*** resultant PVPx/PAM hydrogels exhibit unique phase separation induced by the hydrogen bonding between PVP and PAM and affected by the amount of substance of ***,the phase separation of PVPx/PAM hydrogels results in excellent mechanical properties with a strain of 2590%,tensile strength of 0.28 MPa and toughness of 2.17 MJ/m^(3).More importantly,the hydrogen bonding between PVP and PAM firstly disrupts to dissipate energy under external forces,so the PVPx/PAM hydrogels exhibit good self-recovery properties and outperform chemically cross-linked PAM hydrogels in impact resistance and damping *** is believed that the PVPx/PAM hydrogels with hydrogen-bonding induced phase separation possess more potential application prospects.

关键词： Tough Semi-interpenetrating networks Polyvinylpyrrolidone/polyacrylamide Hydrogels Phase separation

Impact of Carbon Chain Structures in the Backbone on the Flexibility of Modified Polyarylene Sulfide Resins: Molecular Dynamics Simulations and Mesoscopic Analysis

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Chinese Journal of Polymer Science 2024年第4期42卷 544-557页

作者： Chi Zhang Rong Liu Jing-Yuan Liu Wen-Wei Jiang Key laboratory of Fine Chemical engineering and Functional Materials School of Chemical EngineeringSichuan UniversityChengdu610065China

In the domain of high-performance engineering polymers, the enhancement of mechanical flexibility in poly(phenylene sulfide) (PPS) resins has long posed a significant challenge. A novel molecular structure, designated as PP-He-IS, wherein imide rings and an aliphatic hexylene chain are covalently incorporated into the PPS backbone to enhance its flexibility, is introduced in this study. Molecular dynamics (MD) simulations are employed to systematically explore the effects of diversifying the backbone chain structures by substituting phenyl units with alkyl chains of varying lengths, referred to as PP-A-IS where “A” signifies the distinct intermediary alkyl chain configurations. Computational analyses reveal a discernable decrement in the glass transition temperature (Tg) and elastic modulus, counterbalanced by an increment in yield strength as the alkyl chain length is extended. Notably, the PP-He-IS variant is shown to exhibit superior yield strength while simultaneously maintaining reduced elastic modulus and Tg values, positioning it as an advantageous candidate for flexible PPS applications. Mesoscopic analyses further indicate that structures such as PP-He-IS, PP-Pe-IS, and PP-Bu-IS manifest remarkable flexibility, attributable to the presence of freely rotatable carbon-carbon single bonds. Experimental validation confirms that a melting temperature of 504 K which is lower than that of conventional PPS, and lower crystallinity are exhibited by PP-He-IS, thereby affording enhanced processability without compromising inherent thermal stability. Novel insights into the strategic modification of PPS for mechanical flexibility are thus furnished by this study, which also accentuates the pivotal role played by molecular dynamics simulations in spearheading high-throughput investigations in polymer material modifications.

关键词： Molecular dynamics simulations Polyarylene Sulfide Main-chain modifications Flexibility Aliphatic hexylene chain

Palladium-Catalyzed anti-Markovnikov Halosulfonamidation of Unactivated Alkene

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Chinese Journal of Chemistry 2024年第5期42卷 464-470页

作者： Bowen Wang Jianxiao Li Wanqing Wu Huanfeng Jiang State Key laboratory of Pulp and Paper engineering Key Laboratory of Functional Molecular Engineering of Guangdong ProvinceSchool of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhouGuangdong510641 China

Palladium-catalyzed regioselective amination of unactivated alkene remains a challenge and is of great ***,a three-component coupling of unactivated alkene,sulfonamide,and N-halo compounds accessing vicinal haloamine has been *** aminohalogenation represents a modular and regioselective *** electrophilic halogenating agent enables regioselective anti-Markovnikov aminopalladation and facilitates subsequent halogenation *** this protocol is characterized by gram-scale syntheses and late-stage *** note,the recovered byproduct phthalimide allows for reusing by conversion to the starting material.

关键词： Unactivated alkene anti-Markovnikov aminopalladation Vicinal haloamine Palladium catalysis Halosulfonamidation Selectivity N-Halo compounds

Phase-modulated multi-foci microscopy for rapid 3D imaging

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Photonics Research 2024年第7期12卷 1548-1555页

作者： WEIQI WANG LI GONG ZHIWEI HUANG Optical Bioimaging laboratory Department of Biomedical EngineeringCollege of Design and EngineeringNational University of SingaporeSingapore 117576Singapore

3D imaging technology is pivotal in monitoring the functional dynamics and morphological alterations in living cells and ***,conventional volumetric imaging associated with mechanical z-scanning encounters challenges in limited 3D imaging speed with inertial ***,we present a unique phase-modulated multifoci microscopy (PM^(3)) technique to achieve snapshot 3D imaging with the advantages of extended imaging depths and adjustable imaging intervals between each focus in a rapid *** accomplish the tasks,we utilize a spatial light modulator (SLM) to encode the phases of the scattered or fluorescence light emanating from a volumetric sample and then project the multiple-depth images of the sample onto a single charge-coupled device camera for rapid 3D *** demonstrate that the PM^(3)technique provides~55-fold improvement in imaging depth in polystyrene beads phantom compared to the depth of field of the objective lens ***^(3)also enables the real-time monitoring of Brownian motion of fluorescent beads in water at a 15 Hz volume *** precisely manipulating the phase of scattered light on the SLM,PM^(3)can pinpoint the specific depth information in living zebrafish and rapidly observe the 3D dynamic processes of blood flow in the zebrafish *** work shows that the PM^(3)technique developed is robust and versatile for fast 3D dynamic imaging in biological and biomedical systems.

关键词： alterations scattered beads

Electrospun nanofibrous membranes with antimicrobial activity for air filtration

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Chinese Chemical Letters 2024年第10期35卷 173-183页

作者： Guangyao Wang Zhitong Xu Ye Qi Yueguang Fang Guiling Ning Junwei Ye State Key laboratory of Fine Chemicals and School of Chemical engineering Dalian University of Technology engineering laboratory of Boric and Magnesic Functional Material Preparative and Applied Technology

Air pollution, including airborne pathogens and particulate matter(PM), has become a prominent issue affecting human health and safety. Conventional air filtration materials do not meet the requirements for efficient PM capture or do not instantly kill pathogens, leading to increased risk of direct/indirect contact transmission and infection due to the accumulation of pathogens during filtration. Electrospun nanofibrous membranes have emerged as a promising platform due to their rich porous structure, finer fiber diameters, good internal connectivity, and the ability to easily incorporate active chemicals for antimicrobial function. In this review, antimicrobial mechanisms of nanofibrous membranes for air filtration and PM capture mechanisms of nanofibers were firstly investigated, and various types of electrospun nanofibrous membranes with different antimicrobial agents for efficient air filtration were described in detail,including organic antimicrobial agents, inorganic antimicrobial agents and metal-organic frameworks. We hope this work could provide a better practical insight for designing novel electrospun nanofibrous membranes with antimicrobial efficacy for efficient air filtration.

关键词： Air filtration Antimicrobial Electrospinning Nanofibrous membrane Particulate matter

Time-of-flight resolved stimulated Raman scattering microscopy using counter-propagating ultraslow Bessel light bullets generation

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Light(Science & Applications) 2024年第7期13卷 1427-1440页

作者： Shulang Lin Li Gong Zhiwei Huang Optical Bioimaging laboratory Department of Biomedical EngineeringCollege of Design and EngineeringNational University of SingaporeSingapore 117576Singapore

We present a novel time-of-flight resolved Bessel light bullet-enabled stimulated Raman scattering(B2-SRS)microscopy for deeper tissue 3D chemical imaging with high resolution without a need for mechanical *** accomplish the tasks,we conceive a unique method to enable optical sectioning by generating the counterpropagating pump and Stokes Bessel light bullets in the sample,in which the group velocities of the Bessel light bullets are made ultraslow(e.g.,vg≈0.1c)and tunable by introducing programmable angular dispersions with a spatial light *** theoretically analyze the working principle of the collinear multicolor Bessel light bullet generations and velocity controls with the relative time-of-flight resolved detection for SRS 3D deep tissue *** have also built the B2-SRS imaging system and present the first demonstration of B2-SRS microscopy with Bessel light bullets for 3D chemical imaging in a variety of samples(e.g.,polymer bead phantoms,biological samples such as spring onion tissue and porcine brain)with high *** B2-SRS technique provides a>2-fold improvement in imaging depth in porcine brain tissue compared to conventional SRS *** method of optical sectioning in tissue using counter-propagating ultraslow Bessel light bullets developed in B2-SRS is generic and easy to perform and can be readily extended to other nonlinear optical imaging modalities to advance 3D microscopic imaging in biological and biomedical systems and beyond.

关键词： Bessel resolved propagating

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