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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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Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing 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 Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron *** hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of ***,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to *** and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing *** results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

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Sequence design in terpolymerization ofε-caprolactone,CO_(2) and cyclohexane oxide:Random ester-carbonate distributions lead to large-span tunability

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chinese Chemical Letters 2024年第5期35卷 259-264页

作者： Zhenjie Yang Chenyang Hu Xuan Pang Xuesi Chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

It is of great interest to make a degradable material widely tailorable to replace petroleum-derived products among diverse ***,we report the construction of a new multi-purpose degradable material for the first time via a simple ternary copolymerization system comprisingε-caprolactone(ε-CL),cyclohexane oxide(CHO)and CO_(2).Under low pressure of 1 bar∼5 bar,the ring-opening polymerization(ROP)ofε-CL and ring-opening copolymerization(ROCOP)of CO_(2) and CHO can simultaneously *** carbonate units are randomly distributed on the polymer *** random terpolymers have controllable molar mass(10-106 kDa)and compositions(4-33 mol%CO_(2)).And the obtained materials show large-span tunability from tough plastic to elastomer and even adhesive.

关键词： Polyesters CO_(2)-derived copolymers Random copolymerization Elastomers Adhesives

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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

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Stabilizing high-efficiency iridium single atoms via lattice confinement for acidic oxygen evolution

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Nano Research 2024年第4期17卷 2492-2498页

作者： Yibo Wang Jiadong Jiang Zhaoping Shi Hongxiang Wu Jiahao Yang Pengbo Wang Shuai Hou Meiling Xiao Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026.China State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Key Laboratory of Physics and Technology for Advanced Batteries Ministry of EducationCollege of PhysicsJilin UniversityChangchun 130012China

Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined *** optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic *** high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd ***,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.

关键词： lattice confinement iridium single atoms ultralow iridium loading acidic oxygen evolution proton exchange membrane water electrolysis

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Introducing urea into tirapazamine derivatives to enhance anticancer therapy

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National Science Review 2024年第4期11卷 245-253页

作者： Yajun Xu Jianlin Lv Chaoying Kong Ya Liu Kun Wang Zhaohui Tang 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

Tirapazamine（TPZ） has been approved for multiple clinical trials relying on its excellent anticancer ***,as a typical hypoxia-activated prodrug（HAP）,TPZ did not exhibit survival advantages in Phase Ⅲ clinical trials when used in combination therapy due to the insufficient hypoxia levels in patients' *** this study,to improve the therapeutic effects of TPZ,we first introduced urea to synthesize a series of urea-containing derivatives of *** urea-containing TPZ derivatives showed increased hypoxic cytotoxicity（9.51-30.85-fold） compared with TPZ,while maintaining hypoxic ***,one of these derivatives,showed 20-fold higher cytotoxicity than TPZ while maintaining a similar hypoxic cytotoxicity *** highly efficiently deliver TPZP to the tumors and reduce its side effects on healthy tissues,we further prepared TPZP into a nanodrug with fibrin-targeting ability:***4-NPs,a vascular disrupting agent,was used to increase the fibrin level within tumors and exacerbate tumor *** being combined with CA4-NPs,FT11-TPZP-NPs can accumulate in the hypoxia-aggravated tumors and activate sufficiently to kill tumor *** a single-dose treatment,FT11-TPZP-NPs+CA4-NPs showed a high inhibition rate of 98.1% against CT26 tumor models with an initial volume of ～480 mm3and four out of six tumors were completely eliminated;it thereby exerted a significant antitumor *** study provides a new strategy for improving the therapeutic effect of TPZ and other HAPs in anticancer therapy.

关键词： tirapazamine vascular disrupting agent hypoxia-activated prodrug combretastatin A4 urea

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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_(23)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 29 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

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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 18.34,21.73,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

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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

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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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