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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3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 2.%–2.% 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

Degradation mechanisms and stabilization strategies of ruthenium-based catalysts for OER in the proton exchange membrane water electrolyzer

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Progress in Natural Science:Materials International 2024年第1期34卷 207-222页

作者： Ming Yang Hongxiang Wu Zhaoping Shi Yibo Wang Jiahao Yang Jing Ni Pengbo Wang Yuqing Cheng Ziang Wang Meiling Xiao Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of applied chemistry and Engineering University of Science and Technology of China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Designing economical oxygen evolution reaction(OER) electrocatalysts with high activity and long-term stability is essential to promote the scale-up applications of proton exchange membrane water electrolyzer(PEMWE) for hydrogen production. Ruthenium(Ru)-based materials with high intrinsic activity are hailed as the most promising catalysts, but still infeasible for practical application considering their long unresolved poor stability(only dozens of lifespan). Thus, tremendous efforts have been devoted to uncovering the degradation mechanisms and developing stabilization strategies for the Ru-based catalysts. In this review, starting from summarizing the fundamental understanding of deactivation mechanisms, a picture of the stability issue of Ru-based catalysts is proposed, which is followed by a detailed discussion on the recently developed strategies and progress made on enhancing durability. Finally, insights on the prospects for the future development of stable and practical Rubased OER catalysts are provided.

关键词： OER Ru-based catalysts PEMWE Degradation mechanisms Stabilization strategies

Vacancy engineering induced reaction kinetics enhancement of cobalt metaphosphate for pH-universal hydrogen evolution

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Nano Research 2024年第5期17卷 3879-3887页

作者： Yuting Chen Tian Meng Zhicai Xing Yueying Yan Yang Yang Bohan Yao Dewen Wang Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Developing efficient pH-universal hydrogen evolution reaction(HER)catalysts is critical in the field of water electrolysis,however,which is severely hampered by the sluggish kinetics in alkaline ***,a ruthenium(Ru)incorporation induced vacancy engineering strategy is firstly proposed to precisely construct oxygen vacancy(V_(O))-riched cobalt-ruthenium metaphosphate(CRPO)for high-efficiency pH-universal *** V_(O) modifies the electronic structure,improves the superficial hydrophilic and gas spillover capacity,it also reduces the coordination number of Ru atoms and regulates the coordination *** calculations indicate that Ru tends to adsorb H_(2.O and H^(*),whereas V_(O) tends to adsorb OH^(-),which greatly promotes the H_(2.O adsorption and the dissociation of HO-H ***,CRPO-2.exhibits remarkable HER performance,the mass activity is about 18.34,2..73,and 38.07 times higher than that of Pt/C in acidic,neutral,and alkaline media,respectively,at the same time maintain excellent *** findings may pave a new avenue for the rational design of electrocatalysts toward pH-universal water electrolysis.

关键词： cobalt metaphosphate pH-universal hydrogen evolution reaction(HER) vacancy engineering low-coordination atoms oxygen vacancy

Using vitamin C to improve both performance and stability of n-type organic semiconductors

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Science China Materials 2024年第11期67卷 3755-3756页

作者： Sizhe Liu Xingxin Shao Jun Liu Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences School of applied chemistry and Engineering University of Science and Technology of China

Organic semiconductors(OSCs) have the great advantages of flexibility, light weight, low-cost and large-area processing [1].After intensively studied for several decades, OSCs are now considered to be the most promising candidate materials for next-generation electronic circuits. N-type OSCs are the vital component for the basic electronic element, such as p-n junctions, light-emitting diodes and complementary circuits [2..

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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

Highly Red Emissive Conjugated Homopolymers Based on Double B←N Bridged Bipyridine Unit

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Chinese Journal of Polymer Science 2024年第8期42卷 1029-1037页

作者： Yu-Yue Gao Kai-Yuan Zhang Shu-Meng Wang Hui Tong Jun Liu 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

Conjugated homopolymers based on six-member rings,e.g.,polyfluorene,always exhibit blue emission and conjugated homopolymers based on five-member rings,e.g.,polythiophene,can give red emission with low *** this work,we report a series of new conjugated homopolymers based on six-member rings with high-efficiency deep-red *** repeating units of the red light emitting homopolymers are double B←N bridged bipyridine(BNBP)with the boron atoms functionalized with diphenyl,borafluorene,and 2.7-di-tert-butyl-borafluorene groups,*** relationship between the chemical structures and the opto-electronic properties of the monomers and the homopolymers has been systematically *** three polymers emit pure red light(λ_(max)=656 nm)or deep red light(λ_(max)=693 nm)with fluorescence quantum efficiency in solution higher than 60%.The polymers can be used as the emitters in solution-processed organic light-emitting diodes with red emission and decent device *** work indicates a new strategy to design highly efficient light emitting conjugated polymers.

关键词： Conjugated homopolymers Double B←N bridged bipyridine(BNBP) Deep-red emission High fluorescent efficiency

Atomic-level coupled RuO_(2./BaRuO_(3) heterostructure for efficient alkaline hydrogen evolution reaction

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Journal of Energy chemistry 2024年第1期88卷 356-362,I0009页

作者： Yueying Yan Tian Meng Yuting Chen Yang Yang Dewen Wang Zhicai Xing Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina

The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of *** this study,RuO_(2./BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of *** RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2.and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 2. mV of degradation in overpotential after 2.0 h of stability testing at 10 mA cm^(-2..Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water *** research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.

关键词： Heterostructure Hydrogen evolution reaction Interfacial electron transfer Oxygen vacancies

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor *** the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient ***,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)*** lattice disorder in HEOs is believed to increase migration energy barrier of lattice *** a result,the screened Ti_(2.)Nb_(9)Hf_(13)W_(12.Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 2. times lifespan extension compared with the state-of-the-art RuO_(2. *** work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

Preparation of Chemically Recyclable Poly(ether-alt-ester) by the Ring Opening Polymerization of Cyclic Monomers Synthesized by Coupling Glycolide and Epoxides

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Chinese Journal of Polymer Science 2024年第2期42卷 168-175,I0006页

作者： Feng Ren Zhuang-Zhuang Liang Ming-Xin Niu Chen-Yang Hu Xuan Pang Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei230026China

Polyester and polyether are two key oxygenated polymers, and completely alternative sequence of poly(ester-alt-ether) could efficiently combine the advantages(including flexibility, degradability, etc.) of both segments. Currently, despite their copolymers could be synthesized from one-pot mixture of cyclic esters and epoxides, perfectly alternative microstructure is very challenging to realize and typically restricted to certain monomer pairs. Moving forward, synthesizing poly(ester-alt-ether) from commercially available and largescale monomers would be a significant advance. For example, successfully commercialized poly(glycolic acid)(PGA), which is not easily soluble in polymers due to its high crystallinity and is brittle and difficult to control the degradation cycle, would encounter a new paradigm if engineered into poly(ester-altether). In this work, starting from the design of monomer with hybrid structures, we successfully synthesized a series of 1,4-dioxan-2.one containing different substituents based on glycolide(GA) and epoxides using commercially available Salen-Cr(III) and PPNCl catalytic *** new monomers underwent ring-opening polymerization(ROP) to form a series of poly(ester-alt-ether) with perfectly alternating glycolic acid and propylene glycol repeat units under catalytic system of thiourea/base. The poly(ester-alt-ether) have significantly lower glass-transition temperature than PGA. Additionally, the poly(ester-alt-ether) can be chemically recovered to monomer using Sn(Oct)2.or 1,8-diazabicyclo[5.4.0]undecane-7-ene(DBU) as a catalyst in solution, thus establishing a closed-loop life cycle. From monomers derived from GA and epoxides, this work furnishes a novel strategy for the synthesis of poly(ester-alt-ether) with chemical recyclability.

关键词： Polyester Polyether Alternative copolymer Ring-opening polymerization