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Highly efficient room temperature phosphorescent liquid crystalline polymer optical waveguides for advanced optoelectronics

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Science China chemistry 2024年第10期67卷 3450-3457页

作者： Jie Li Yan Guan Wei Xia Jin-Kang Chen Jiang Huang Yi Chen Qi Lin Er-Qiang Chen He-Lou Xie Key Laboratory of Environmentally Friendly chemistry and Application of Ministry of Education and Key Laboratory of Advanced Functional Polymer Materials of CollegesUniversities of Hunan Province and College of ChemistryXiangtan University Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking University School of physics and Optoelectronics Xiangtan University

Active organic optical waveguide materials(OOWMs) incorporating room temperature phosphorescence(RTP) hold significant promise for diverse applications in photonic and optoelectronic devices. Despite this potential, realizing active RTP optical waveguides with large-sized ordered structures and minimal light loss remains a formidable challenge. To address this issue, we present a groundbreaking thermoplastic active OOWM with low light loss, leveraging room temperature phosphorescent liquid crystalline polymer(LCP). This innovative material can be easily synthesized through the copolymerization of phosphorescent and liquid crystalline monomers. The resulting RTP copolymer exhibits a nematic liquid crystal phase with a phosphorescence lifetime of approximately 0.15 ms and an afterglow duration of around 1 second. Leveraging the excellent processability of LCP,we successfully produce meter-scale fibers via melt spinning. These RTP LCP fibers, characterized by a high orientation of mesogens along the fiber axis, demonstrate superior light confinement and efficient light conduction compared to unoriented samples, resulting in a low optical loss coefficient of 0.13 dB/mm. Furthermore, the thermal responsiveness of the RTP LCP optical waveguide enables its use as a photo switch. This pioneering work paves the way for the design of new OOWMs tailored for advanced photonics and optoelectronics devices.

关键词： room temperature phosphorescence liquid crystalline polymer active optical waveguide

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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

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Open-Shell Oligomers and polymers: Theory, Characterization Methods, Molecular Design, and Applications

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Chinese Journal of polymer Science 2024年第4期42卷 417-436页

作者： Xue-Qing Wang Cheng Song Ting Lei Key Laboratory of polymer chemistry and physics(Ministry of Education) School of Materials Science and EngineeringPeking UniversityBeijing100871China

Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFETs), photodetectors, organic thermoelectrics, and spintronics. Although open-shell ground states have been observed in certain small molecules and doped organic semiconductors, the exploration of open-shell ground-state conjugated polymers is still limited, and the strategies for designing these polymers remain obscure. This review aims to briefly introduce the theory and characterization methods of open-shell conjugated polymers, along with an overview of recent progress and applications. The objective is to stimulate further advancements and investigations in this promising area by shedding light on the potential of open-shell conjugated polymers and the challenges that lie ahead.

关键词： Conjugated polymers Open-shell molecules High-spin ground state Donor-acceptor(D-A)polymers Optoelectronic and magnetic properties

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A High-Performance Electrochemical Analysis Platform for Ultrasensitive Detection of HTLV-1 DNA: Integrating Cascade Signal Amplifi cation with λ-Exonuclease-Assisted Target Recycling and Enzyme Catalysis

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Journal of Analysis and Testing 2024年第03期8卷 361-373页

作者： Qi Xiao Shuai Liu Yali Wang Huihao Li Mingli Yang Yi Fang Sijing Chen Shan Huang Guangxi Key Laboratory of Natural polymer chemistry and physics College of Chemistry and Materials Nanning Normal University

Human T-cell lymphophilic virus type 1 (HTLV-1), the known retrovirus causing cancer in humans, is closely associated with adult T-cell leukemia/lymphoma and HTLV-1 associated myelopathy/tropical spastic paraparesis. Due to its ability to evade the host's defense mechanisms, early tracking of HTLV-1 becomes crucial. In this study, we integrateλ-Exonuclease(λ-Exo)-assisted target recycling with a terminal deoxynucleotidyl transferase (TdT)-mediated template-free DNA extension process to develop an electrochemical analysis platform for the specifi c and sensitive detection of HTLV-1 DNA. During theλ-Exo-assisted target recycling, HTLV-1 DNA is recognized by hairpin DNA (Hp-DNA), forming double-stranded DNA(dsDNA) through DNA hybridization. The dsDNA, featuring blunt 5'terminal phosphorylation, is cleaved byλ-Exo, generating abundant short output sequence (sDNA). HTLV-1 DNA is released, initiating a cyclic hybridization-cleavage ***, thiol-labelled capture DNA (CP-DNA) assembled on gold electrode surface captures a substantial amount of the generated sDNA, forming CP-DNA-sDNA nanostructures. When TdT and dNTPs are present on the electrode surface, the3'-OH terminal of sDNA extends to generate long single-stranded DNA (ssDNA) structure. Methylene blue (MB) is selected as the electrochemical signal molecule. MB not only binds with ssDNA but also interacts specifi cally with dsDNA, resulting in a signifi cantly enhanced electrochemical signal on modifi ed electrode surface. The detection limit of HTLV-1 DNA is as low as 19 amol/L (S/N=3) when the two signal amplifi cation strategies are combined. The analysis platform exhibits excellent analytical performance and holds promise as a novel tool for the early tracing and diagnosis of HTLV-1 DNA.

关键词： Cascade signal amplification Electrochemical DNA sensor Enzyme-assisted target recycling HTLV-1 DNA

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Linear Viscoelasticity of ABA-type Vitrimer Based on Dioxaborolane Metathesis

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Chinese Journal of polymer Science 2024年第10期42卷 1495-1504页

作者： Shi-Long Wu Huan-Huan Yang Quan Chen State Key Laboratory of polymer physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Science University of Science and Technology of China

In this study, we synthesized a series of ABA-type vitrimers by crosslinking the short A moieties of precursors with a bifunctional crosslinker and evaporating the small molecular byproduct. The vitrimer samples thus prepared exhibit linear viscoelasticity dependent on the length of A moiety as well as the content of the crosslinks. When the average number of A monomers per end moiety m=1.1, the crosslinker can only extend the chain but not crosslink the chain. When m becomes 2.8 or higher, introducing a crosslinker first leads to the gelation, whereas excess in crosslinker molecules leads opening of the crosslinking sites and accordingly reentry into the sol regime. Surprisingly, a further increase in the length of the A moieties increases the relaxation time much weaker than the exponential increase seen for the physically crosslinked ABAtype ionomers. We attribute this difference to the distinct relaxation mechanisms:the relaxation of the vitrimer samples is based on relatively independent exchange reactions, which contrasts with the ABA-type ionomers that relax through the collective hopping of connected ionic groups from one ion aggregate to another.

关键词： ABA-type vitrimer Kinetics and thermodynamics Linear viscoelasticity polymer rheology Relaxation mechanism

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Critical Role of Ethylene-Propylene Block Copolymer in Impact Polypropylene Copolymer

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Chinese Journal of polymer Science 2024年第3期42卷 344-351,I0007页

作者： Yu-Hui Tang Na Zhang Wei Bao Wei Jiang Yuan Lin Zhao-Hui Su State Key Laboratory of polymer physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Ethylene-propylene block copolymer(EbP) is a vital component in impact polypropylene copolymer(IPC), yet its distribution in the multiphase composite material and how it influences the phase structure and the mechanical properties are not well understood. In this work,four IPCs were investigated by atomic force microscopy-infrared(AFM-IR) to assess the phase compositions in situ, based on which in conjunction with the chain microstructure information obtained ex situ the distributions of the copolymer components were derived for each alloy. For the IPCs whose EbP comprises long P and long E segments, the EbP fraction was found to phase separate from the rubber and the PP matrix to form the cores of the disperse particles with the E-P segmented copolymer(EsP). In contrast, in the IPC with EbP composed of long P and short E segments, the EbP fraction formed an outer shell for the rubber particles with the cores comprising the EsP alone, and this IPC, containing a lower E comonomer content than its counterpart, exhibited both better impact resistance and higher flexural modulus. These results clarify how the chain structure of EbP governs the phase morphology in IPC, which in turn impacts the properties of the composite material.

关键词： Impact polypropylene copolymers AFM-IR Ethylene-propylene block copolymers Core-shell rubber particles

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Polyoxometalate-based flexible conductive materials with superionic conductivity

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Science China chemistry 2024年第10期67卷 3299-3309页

作者： Yuxin Wang Shuping Xue Jun Geng Ying Lu Teng Li Xiaozheng Duan Xue Bai Yanli Yang Jingqi Yang Shuxia Liu Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education College of ChemistryNortheast Normal University State Key Laboratory of polymer physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences

Flexible ion-conductive materials exhibit intriguing advantages for applications in flexible electronic ***,the further enhancement of their conductivity within environmental limitations is an urgent demand for the development of flexible electronic devices,yet remains as a great ***,we report a“dual-acid”strategy,via the encapsulation of two acids,H3PW12O40（HPW） and NH2SO3H（SA）,with synergistic interaction into poly（vinyl alcohol）-glycerol（PVA-Gly） hydrogel,to achieve polyoxometalate（POM）-based flexible materials with superionic conductivity under various environmental *** a representative example,the prepared PVA-Gly/HPW-SA-20% hydrogel presents an ultrahigh proton conductivity ranging from -30℃(3.33×10-2S cm-1) to room temperature(2.78×10-1S cm-1) under ambient ***,the PVA-Gly/HPW-SA-20% hydrogel exhibits remarkable advantages in anti-freezing,mechanical flexibility and self-adhesiveness,making it a promising multifunctional electrolyte for flexible electronic *** experimental results and molecular dynamics（MD） simulations jointly demonstrate that SA bridges HPW clusters to form a dense proton transport pathway induced by multiple electrostatic and hydrogen bonding interactions between SA and HPW counterparts,which contributes to the high-level proton conductivity of the PVA-Gly/HPW-SA-20% *** work provides new insights into the design of POM-based flexible materials with superionic conductivity.

关键词： polyoxometalates proton conduction dual-acid effect hydrogel molecular dynamics simulation

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Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第03期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen Key Laboratory of polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research Institute Chinese Academy of Agricultural Sciences Jilin Biomedical polymers Engineering Laboratory State Key Laboratory of polymer physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2

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An n-type organoboron polymer for red-light-selective organic photodetectors

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Science Bulletin 2024年第16期69卷 2501-2504页

作者： Xu Cao Hongkun Tian Lu Zhang Jun Liu Lixiang Wang State Key Laboratory of polymer physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Color-selective light detection is required for high-resolution imaging,optical communication,biomedical applications,and so on[1,2].Typical photodetectors using broad-band absorption materials as the active layers exhibit wide photoresponse *** general strategy for color-selective light detection is to use additional optical *** integration of photodetectors and optical filters inevitably increases device complexity and manufacturing ***,scientists have demonstrated some device design strategies for color-selective photodetectors and narrow photoresponse spectra have been achieved[3].

关键词： light selective boron

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Comparison of Measurements for Enhanced Diffusion Problem in Chemical Reaction Systems

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Chinese Journal of chemistry 2024年第14期42卷 1659-1664页

作者： Ah-Young Jee Ziyang Wen Huan Wang Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringBeijing Key Laboratory of Polymer Chemistry&Physics of Ministry of EducationPeking UniversityBeijing100871 China

The problem of molecular diffusion in the soup of chemical reactions attracts mounting interest across fields ranging from chemistry to biophysics to material *** reactions involve bond breakup and formation,whose time scale is typically on the orders of fs to ps,while molecular diffusion occurs at time scales ofμs to *** two processes are often considered orthogonal,given the vastly different *** serial results show that the enzyme's diffusion is enhanced in a substrate-dependent manner,which was further extended to small molecule reaction systems,challenging this classical ***,the results from different groups using different techniques do not quantitatively agree,and a general mechanism is yet to be *** summarize experimental studies on diffusion problems and seek to reconcile the interpretation with understanding the limits of measurement tools and the chemical nature of reaction *** molecular diffusion in chemical reactions will provide fresh thoughts in designing chemical systems such as molecular machines that harvest work at the nanoscale in a controllable manner.

关键词： Molecular diffusion Chemical reactions Enzyme reactions Active matter Diffusion measurements Single-molecule studies Fluorescence Time-resolved spectroscopy

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