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Multiscale control of MnO_(2) growth via[WO_(6)]-perturbed[MnO_(6)]assembly toward a favorable balance between capacitance and rate performance

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Rare Metals 2024年第4期43卷 1658-1671页

作者： Jin-Kang Liu Tian-Shuo Yang Zhi-Bin Ren Adekunle-Adedapo Obisanya Xin-Yi Tan Yan-Di Rao Jun-Shuang Zhou Fa-Ming Gao Jian-Ren Wang Hebei Key laboratory of applied chemistry Yanshan UniversityQinhuangdao066004China

Although pseudocapacitive manganese dioxide(MnO_(2))integrates the high-power merit of carbonaceous materials with the high-energy merit of battery-type materials,it still has a long way to go in achieving a more satisfactory balance of higher energy and power density,and in decoupling the relationship of structural characteristics with energy storage *** realize such goals,a bottom-up[WO_(6)]-perturbed[MnO_(6)]assembly strategy has been developed here due to their similar structure,yet mismatched lattice *** facile protocol is capable of finely controlling the morphology and crystal structure of MnO_(2)by adjusting its internal[WO_(6)]***,the as-prepared W_xMnO_(2)is treated as an ideal platform to scrutinize the correlations of the structure with the energy storage *** operando Raman spectra and finite element analysis have fully demonstrated the superiority of the locally ordered defects-enriched structure of W_(0.02)-MnO_(2),which could reach a favorable balance between the ion diffusion equilibrium time and the number of active *** a result,the W_(0.02)-MnO_(2)is able to deliver a high capacitance of 292 F·g^(-1)at a current density of 1 A·g^(-1)and a remarkable rate performance with a 60%capacity retention at a current density of 50 A·g^(-1).The further unveiled structure-performance relationship provides a guideline for the design of better pseudocapacitive energy storage devices.

关键词： Supercapacitors Pseudocapacitive materials MnO_(2) Tungsten doping Crystal structure regulation

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 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

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

Ligand-controlled NiH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science China chemistry 2024年第6期67卷 1935-1940页

作者： Ya-Ping Shao Zhuo-Min Chi Yong-Min Liang State Key laboratory of applied Organic chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor *** method enables the synthesis of diverseβ-orγ-branched aromatic *** mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable ***,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： NiH regiodivergent hydroalkylation azaarenes interrupted chain-walking

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Synergistic enhancement of ultrasound therapy for tumors using hypoxia-activated 6-diazo-5-oxo-L-norleucine(DON)prodrug nanoparticles

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Nano Research 2024年第7期17卷 6323-6331页

作者： Mengfei Zheng Zhilin Liu Hang Xu Daping Ye Linjie Cui Chenguang Yang Lili Ma Kun Wang Kazuo Sakurai Zhaohui Tang Key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Jilin Biomedical Polymers Engineering laboratory Changchun 130022China Department of chemistry and biochemistry The University of Kitakyushu1-1 HibikinoKitakyushu 808-0135Japan

Ultrasound(US)has been applied in clinical practice for its non-invasive and high ***,it is difficult to achieve a satisfactory anti-tumor effect with US ***,the use of US therapy alone can exacerbate tumor *** this study,we prepared hypoxia-activated 6-diazo-5-oxo-L-norleucine(DON)prodrug nanoparticles(HDON-NPs)to improve US therapeutic *** an H22 murine liver cancer model,US therapy selectively disrupted tumor blood vessels,leading to increased tumor hypoxia and a 1.67-fold increase in the expression of nitroreductase(NTR).The combination therapy of US and HDON-NPs demonstrated a synergistic effect,resulting in a tumor suppression rate(TSR)of 90.2%±6.4%,which was 5.93-fold higher than that of US therapy *** combined treatment selectively blocked the glutamine metabolism of the tumor cells while simultaneously activating the T cells in the tumor microenvironment,thereby exerting a robust anti-tumor effect.

关键词： ultrasound therapy hypoxia-activated prodrug nanoparticles 6-diazo-5-oxo-L-norleucine(DON) glutamine antagonist starvation therapy

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

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.

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 25 mV of degradation in overpotential after 200 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

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