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Surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

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Uncovering the dominant contribution of intermediate volatility compounds in secondary organic aerosol formation from biomass-burning emissions

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National Science Review 2024年第3期11卷 150-158页

作者： Kun Li Jun Zhang David M.Bell Tiantian Wang Houssni Lamkaddam Tianqu Cui Lu Qi Mihnea Surdu Dongyu Wang Lin Du Imad El Haddad Jay G.Slowik Andre S.H.Prevot Environment Research institute Shandong University Laboratory of Atmospheric chemistry Paul Scherrer Institute

Organic vapors from biomass burning are a major source of secondary organic aerosols(SOAs). Previous smog chamber studies found that the SOA contributors in biomass-burning emissions are mainly volatile organic compounds(VOCs). While intermediate volatility organic compounds(IVOCs) are efficient SOA precursors and contribute a considerable fraction of biomass-burning emissions, their contribution to SOA formation has not been directly observed. Here, by deploying a newly-developed oxidation flow reactor to study SOA formation from wood burning, we find that IVOCs can contribute ～70% of the formed SOA, i.e.>2 times more than VOCs. This previously missing SOA fraction is interpreted to be due to the high wall losses of semi-volatile oxidation products of IVOCs in smog chambers. The finding in this study reveals that SOA production from biomass burning is much higher than previously thought, and highlights the urgent need for more research on the IVOCs from biomass burning and potentially other emission sources.

关键词： atmospheric chemistry biomass burning secondary organic aerosol intermediate volatility organic compounds

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p-wave resonances in the exponential cosine screened Coulomb potential

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Communications in Theoretical Physics 2024年第7期76卷 105-113页

作者： Yuan-Cheng Wang Li Guang Jiao Aihua Liu Yew Kam Ho Stephan Fritzsche College of Physical Science and Technology Shenyang Normal UniversityShenyang 110034China College of Physics Jilin UniversityChangchun 130012China Helmholtz-Institut Jena D-07743 JenaGermany GSI Helmholtzzentrum fur Schwerionenforschung GmbH D-64291 DarmstadtGermany institute of Atomic and Molecular Physics Jilin UniversityChangchun 130012China institute of Atomic and Molecular Sciences Academia SinicaTaipei 10617TaiwanChina

We perform benchmark calculations of the p-wave resonances in the exponentially cosine screened Coulomb potential using the uniform complex-scaling generalized pseudo-spectral *** present results show significant improvement in calculation accuracy compared to previous predictions and correct the misidentification of resonance electron configuration in previous *** is found that the resonance states approximately follow an n^(2)-scaling law which is similar to the bound *** birth of a new resonance would distort the trajectory of an adjacent higher-lying resonance.

关键词： complex-scaling method shape resonance generalized pseudospectral method exponential cosine screened Coulomb potential

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Friction between Strongly Compressed Polymer Brushes

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Chinese Journal of Polymer Science 2024年第9期42卷 1368-1374,I0008页

作者： Qi Liao institute of chemistry Chinese Academy of SciencesBejing 100190China

We present the results of molecular dynamics simulations of steady shear between a pair of neutral polymer brushes,as well as a pair of charged polymer brushes in the strongly compressed *** results of the molecular dynamic simulations of neutral and polyelectrolyte brushes in implicit solvent including normal forces,shear forces,viscosities and friction coefficients as a function of separation between brushes,are presented in the *** comparison of the simulation results of neutral and charged brushes shows that the charged brushes is in the quasi-neutral regime,and the dependence of viscosity on the separation distance show the similar power law of neutral *** simulation results confirm that the implicit solvent simulations of polyelectrolyte brushes that ignore hydrodynamics interaction are in agreement with the scaling predictions qualitatively because of screening of hydrodynamic interaction and long-range electrostatic interactions on the correlation length *** of neutral and charged brushes show the lubrication properties that the friction coefficient decreases with the separation decreases at enough large ***,a maximum of friction coefficients is observed for polyelectrolyte brushes,which is in contrast to the neutral brushes with monotonical dependence.

关键词： Polymer brush Frictions coefficient Polyelectrolyte Lubrication

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Evolution exploration and structure prediction of Keggin-type group IVB metal-oxo clusters

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Chinese Chemical Letters 2024年第5期35卷 487-492页

作者： Run-Han Li Tian-Yi Dang Wei Guan Jiang Liu Ya-Qian Lan Zhong-Min Su School of chemistry South China Normal UniversityGuangzhou 510006China institute of Functional Material chemistry Faculty of ChemistryNortheast Normal UniversityChangchun 130024China institute of Theoretical chemistry Jilin UniversityChangchun 130023China

The fascinating chemical structure and broad application prospect of Keggin-type polyoxometalates(POMs)have attracted many chemists to explore and discover *** the traditional Keggin,larger metal atomic radius,higher metal coordinated numbers,lower metal valence states and other features allow the group IVB metal-based Keggin(IVB-Keggin)more space and unknown in terms of structure and ***,density functional theory(DFT)calculations were performed to explore the influences including cores,shells,caps,and terminal ligands,et *** IVB-Keggin,and analyze the possibility of novel structure *** the perspective of multi-layer onion-like clusters,molecular energy level,host-guest interaction energy,surface charge and covalent bond polarity can be further adjusted to achieve the oriented design of functional *** insights are expected to provide theoretical support for experimental synthesis,opening a new perspective to understand the growth of Keggin.

关键词： Keggin Metal-oxo clusters Group IVB Onion pattern DFT

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The chlorine evolution reaction promoted by organocatalysts with amide functional groups

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Science China chemistry 2024年第3期67卷 749-750页

作者： Lan Zhao Liang-Nian He State Key Laboratory and institute of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

Since the nineteenth century, the chlor-alkali process entails the electrochemical oxidation of sodium chloride solutions to Cl_(2) by the chlorine evolution reaction(CER) and the simultaneous production of sodium hyd... 详细信息

关键词： chlorine hydroxide promoted

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Ink-structing the future of vascular tissue engineering:a review of the physiological bioink design

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Bio-Design and Manufacturing 2024年第2期7卷 181-205页

作者： Judith Synofzik Sebastian Heene Rebecca Jonczyk Cornelia Blume institute for Technical chemistry Leibniz University Hannover30167 HannoverGermany

Three-dimensional(3D)printing and bioprinting have come into view for a plannable and standardizable generation of implantable tissue-engineered constructs that can substitute native tissues and *** tissue-engineered structures are intended to integrate with the patient’s *** tissue engineering(TE)is relevant in TE because it supports the sustained oxygenization and nutrition of all tissue-engineered *** have a specific role,representingthenecessarymedium for printability and vascular cell *** review aims to understand the requirements for the design of vascular ***,an in-depth analysis of vascular cell interaction with their native environment must be gained.A physiological bioink suitable for a tissue-engineered vascular graft(TEVG)must not only ensure good printability but also induce cells to behave like in a native vascular vessel,including self-regenerative and growth *** review describes the general structure of vascular walls with wall-speciﬁc cell and extracellular matrix(ECM)components and biomechanical properties and ***,the physiological role of vascular ECM components for their interaction with vascular cells and the mode of interaction is *** currently available or imaginable bioinks are described from physiological matrix proteins to nonphysiologically occurring but natural chemical compounds useful for vascular *** physiological performance of these bioinks is evaluated with regard to biomechanical properties postprinting,with a view to current animal studies of 3D printed vascular ***,the main challenges for further bioink development,suitable bioink components to create a self-assembly bioink concept,and future bioprinting strategies are *** concepts are discussed in terms of their suitability to be part of a TEVG with a high potential for later clinical use.

关键词： Vascular wall histology Vascular cells Microenvironment Extracellular matrix Cell–matrix interaction Bioink Printability

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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 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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General radical difluoromethylation using difluoroacetic anhydride via photoredox catalysis

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Science China chemistry 2024年第8期67卷 2637-2646页

作者： Meng He Yankai Yang Heng Zhang Zhipeng Guan Zhi-Bing Dong Hong Yi Aiwen Lei School of chemistry and Environmental Engineering Wuhan Institute of TechnologyWuhan 430205China College of chemistry and Molecular Sciences and institute for Advanced Studies(IAS) Wuhan UniversityWuhan 430072China

CF_(2)H-containing molecules play pivotal roles in diverse fields from medicinal chemistry to materials science. However, the application of existing CF_(2)H reagents as a source of CF_(2)H radical is limited by their reactivity and preparation. Herein, we develop a simple and general visible-light-catalyzed radical difluoromethylation reaction of alkenes, dienes, and heteroaromatics using commercially available, easy-to-handle, and low-cost difluoroacetic anhydride as the CF_(2)H reagent. This scalable protocol enables the convenient synthesis of a range of CF_(2)H-containing compounds under mild conditions, exhibiting a broad substrate scope and functional group tolerance. Potential applications are further demonstrated by gram-scale synthesis, sunlight experiments, derivatization experiments as well as the synthesis of bioactive molecules.

关键词： radical difluoromethylation alkenes/dienes/heteroaromatics difluoroacetic anhydride photoredox

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Advancements in synthetic and electrocatalytic exploitation of guest-host intercalated 2D materials

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Progress in Natural Science:Materials International 2024年第3期34卷 454-469页

作者： Qian Yang Kun Wang Meiling Zhang Feihong Du Jiayang Li Chen Zheng Jinyang Li School of chemistry Southwest Jiaotong University Yibin institute of Southwest Jiaotong University

The emergence and development of layered materials have shown great promise for many applications, especially in recent years, the effective modulation of the physicochemical properties of layered materials by intercalation chemistry has led to great potential in material design. In this paper, we review the reaction mechanisms of different guest species(metal atoms/ions, organic molecules/ions, inorganic molecules and inorganic ions)intercalated into the host layered materials as well as the recent progress. It is also reviewed that layered intercalated materials with controllable structure and tunable physicochemical properties can be prepared through the occurrence of interactions between different subjects and guests. The specific applications of intercalation chemistry in the field of electrocatalysis, such as the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction and other electrocatalytic reactions, are then discussed, with emphasis on the mechanism of the improved catalytic activity and stability of the layered materials after guest intercalation.

关键词： Electrocatalysis Guest species Intercalation chemistry Layered materials

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