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Supramolecular Biomaterials for Cancer Immunotherapy

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Research 2024年第2期2023卷 491-509页

作者： Huan Liang Qingqing Lu Jie Yang Guocan Yu College of Science Nanjing Forestry UniversityNanjing 210037P.R.China Key Laboratory of bioorganic Phosphorus chemistry&Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084P.R.China

Cancer immunotherapy has achieved tremendous successful clinical results and obtained historic victories in tumor ***,great limitations associated with feeble immune responses and serious adverse effects still cannot be neglected due to the complicated multifactorial etiology and pathologic microenvironment in *** rapid development of nanomedical science and material science has facilitated the advanced progress of engineering biomaterials to tackle critical *** supramolecular biomaterials with flexible and modular structures have exhibited unparalleled advantages of high cargo-loading efficiency,excellent biocompatibility,and diversiform immunomodulatory activity,thereby providing a powerful weapon for cancer *** past decades,supramolecular biomaterials were extensively explored as versatile delivery platforms for immunotherapeutic agents or designed to interact with the key moleculars in immune system in a precise and controllable *** this review,we focused on the crucial role of supramolecular biomaterials in the modulation of pivotal steps during tumor immunotherapy,including antigen delivery and presentation,T lymphocyte activation,tumor-associated macrophage elimination and repolarization,and myeloid-derived suppressor cell *** on extensive research,we explored the current limitations and development prospects of supramolecular biomaterials in cancer immunotherapy.

关键词： biomaterials limitations thereby

Auxiliary ball milling to prepare WS_(2)/graphene nanosheets composite for lithium-ion battery anode materials

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Tungsten 2024年第1期6卷 124-133页

作者： Yong-Lin Wu Jia-Bin Hong Wei-Xu Zhong Chun-Xiang Wang Zhi-Feng Li Sydorov Dmytro Jiangxi Provincial Key Laboratory of Power Batteries and Materials Jiangxi University of Science and TechnologyGanzhou 341000China Faculty of Materials Metallurgy and chemistry Jiangxi University of Science and TechnologyGanzhou 341000China institute of bioorganic chemistry and Petrochemistry National Academy of Sciences of UkraineKiev 02160Ukraine

A novel nano-WS_(2)/graphene nanosheets(GNSs)composite is obtained by ball milling with xylitol as auxiliary agent and hightemperature *** improves the shear force during ball milling and well overcomes the van der Waals interactions between the interlayer of graphite and WS_(2).Through high-temperature calcination,GNSs and WS_(2) nanosheets can form tight interface *** produced WS_(2)/GNSs composites can be used as anode materials for lithium-ion batteries,while maintaining a high reversible specific capacity of 705 mAh·g^(-1)with the capacity retention of 95%at a current density of 250 mA·g^(-1)after 200 cycles,mainly because WS_(2)/GNSs composites have a higher Li^(+)diffusion coefficient of 2.2×10^(-9)cm^(2)·s^(-1)and a higher specific surface area of 70.10 m^(2)·g^(-1).As a result,the xylitol-assisted ball milling method designed in this work is suitable for extended preparation of peeling of two-dimensional layer materials into nanosheets.

关键词： Lithium-ion battery Anode material WS_(2) Graphene nanosheets Auxiliary ball milling

Cyclic Dinucleotide Self-Assembled Nanoparticles as a Carrier-Free Delivery Platform for STING-Mediated Cancer Immunotherapy

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CCS chemistry 2024年第1期6卷 177-195页

作者： Lang Zhao Shao-Hua Zhuo Tian-Yang Wang Jun-Jun Wu Jing-Yun Su Wen-Hao Li Bo-Dou Zhang Yan-Mei Li Key Lab of bioorganic Phosphorus chemistry&Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084 Beijing institute for Brain Disorders Beijing 100069 Center for Synthetic and Systems Biology Tsinghua UniversityBeijing 100084

Cyclic dinucleotides(CDNs)are natural agonists of the stimulator of interferon genes(STING),which is an attractive immunotherapy ***,CDNs and their derivatives are being investigated ***,the poor bioavailability of exogenous CDNs has limited their application in *** nanocarriers are widely used for cytosolic delivery of CDNs,their loading capacity is insufficient,and their complicated composition and purification process raises bio-compatibility ***,we report a super-simplified CDN self-assembly strategy for carrier-free delivery of *** the presence of excess K^(+),CDNs form oligomers which further self-assemble with divalent metal ions(such as Mn^(2+))to form nanoparticles(NPs)in aqueous *** demonstrate that the self-assembled CDN NPs promote cellular uptake of CDNs and enhance tumor immunogenicity by remodeling the tumor microenvironment,inducing immunogenic tumor cell death and increasing tumorinfiltrating lymphocytes,which is conducive to the generation of tumor neoantigen-specific T-cell *** also demonstrate that the use of CDN NPs alone or in combination with immune checkpoint blockades inhibits tumor growth,highlighting the fact that CDN NPs are a potent platform for cancer immunotherapy.

关键词： cyclic dinucleotide STING carrierfree delivery tumor immunogenicity cancer immunotherapy

Electrocatalytic performance of CNTs/graphene composited rare earth phthalocyanines(M=La,Y,Yb,Sc)

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Journal of Rare Earths 2024年第2期42卷 323-333,I0004页

作者： Tingting Jiang Caixia Ou Luyi Wang Jun Chen Sydorov Dmytro Qian Zhang Jintian Luo Hua Wang Jiangxi Key Laboratory of Power Batteries and Materials Faculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou341000China Joint Department of Electrochemical Energy Systems Institute of Bioorganic Chemistry and PetrochemistryNational Academy of Sciences of Ukraine38A VernadskyAveKiev03142Ukraine Guangdong Jiana Energy Technology Co. Ltd.Qingyuan511500China

In this study,a class of rare earth composite sandwich phthalocyanines(MPcs,M=La,Y,Yb,Sc) were prepared and compounded with graphene and carbon nanotubes to obtain MPc/Gr and MPc/CNTs *** electrocatalytic behaviors of MPc/Gr and MPc/CNTs electrodes were further *** results show that the central rare earth metal has a large influence on the electrocatalytic *** the MPcs/Gr samples,ScPc with the smallest ionic radius and molecular size can be more uniformly dispersed in graphene,and the hydrogen precipitation overpotential of ScPc/Gr electrode is514 mV,corresponding to a Tafel slope of 148 mV/dec,with better electrocatalytic performance than other rare earth metal *** for the MPc/CNTs composites,LaPc,which has the largest ionic radius and molecular size,is more uniformly dispersed on the surface of CNTs,so that the LaPc/CNT electrode exhibits the best LSV performance with the smallest corresponding Tafel slope(176 mV/dec).The main reason is the different binding modes of MPcs molecules in Gr and *** rare earth phthalocyanine is combined with layered graphene,the smallest size of rare earth phthalocyanine(ScPc)is more easily embedded in the graphene layer,resulting in better homogeneity of the composite,larger effective contact area and better electrocatalytic *** contrast,when rare earth phthalocyanine is bound to carbon nanotubes in a tubular structure,it is mainly bound by attaching to the surface or being entangled by the carbon *** this case,the rare-earth phthalocyanine molecules(LaPc)with larger layer spacing can provide more contact area with CNTs,forming a more uniform and effective composite,which eventually provides more active sites and better electrocatalytic performance.

关键词： Electrocatalysis Rare earth phthalocyanines Graphene(Gr) Carbon nanotubes(CNTs) Composite

Effect of Ta_(2)O_(5)nanoparticles on bioactivity,composition,structure,in vitro and in vivo behavior of PEO coatings on Mg-alloy

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Journal of Magnesium and Alloys 2024年第6期12卷 2360-2379页

作者： D.V.Mashtalyar I.M.Imshinetskiy V.V.Kashepa K.V.Nadaraia M.A.Piatkova A.I.Pleshkova K.A.Fomenko A.Yu.Ustinov S.L.Sinebryukhov S.V.Gnedenkov institute of chemistry Far Eastern BranchRussian Academy of SciencesVladivostok690022Russia Far Eastern Federal University Vladivostok690950Russia Regional Clinical Dermatovenerological Dispensary Vladivostok690033Russia

The present study investigates the physical and chemical characteristics,behavior in vitro and in vivo,and biocompatibility of coatings containing Ta_(2)O_(5),which are obtained by plasma electrolytic oxidation(PEO)on MA8 magnesium *** obtained coatings demonstrate in vivo biocompatibility and in vitro *** to the base PEO coating,the layers containing Ta_(2)O_(5)facilitate the development of apatite in simulated body fluid,suggesting that the inclusion of nanoparticles improves bioactivity of the *** was found that incorporation of Ta_(2)O_(5)nanoparticles increases roughness and porosity of the formed layers by increasing particle concentration in electrolytes for the PEO process contributing to sufficient soft tissue ingrowth in *** on in vivo studies,these coatings also provide favorable tissue response and minimal inflammatory reaction in comparison with the bare magnesium alloy due to protection of living tissues from deleterious corrosion events of magnesium implant such as local alkalization and intense hydrogen *** results obtained in the present study concluded biocompatibility,tissue integration of the PEO coatings containing Ta_(2)O_(5)nanoparticles making them a promising protective layer for biodegradable magnesium implants.

关键词： Plasma electrolytic oxidation Bioactive coatings Tantalum pentoxide Simulated body fluid(SBF) Apatite formation Histology

Natural products inspired[3+2]cycloaddition enables efficient construction of hydroxylated tetrahydrofuran acetals and concise syntheses of lignans

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Science China chemistry 2024年第7期67卷 2306-2313页

作者： Dong-Yue Cai Weiming Shi Zhao-Hui Jin Zhi-Xiang Yu Jin-Xin Zhao Jian-Min Yue State Key Laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China University of Chinese Academy of Sciences Beijing 100049China Beijing National Laboratory for Molecular Sciences(BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China

Mimicking biosynthetic pathways of hongkonoids led to the development of a new Cu(Ⅰ)-catalyzed[3+2]cycloaddition ofα-hydroxyketone andβ-keto enol ethers,affording tetrahydrofuran acetals in a highly diastereoselective manner and 100%atom *** studies on the mechanism disclosed a concerted but asynchronous Michael addition/aldol *** the same importance,this methodology provides a practical biomimetic approach for one-step construction of the dibenzylbutyrolactol lignan backbone starting from two phenyl propane derivatives,opening up a powerful new approach for lignan synthesis,which is showcased by succinct total syntheses of two biologically important aryltetralin-type lignans,β-apopicropodophyllin and *** the mild and operationally simple conditions,the developed chemistry might have a promising prospect in potential industrial applications.

关键词： [3+2]cycloaddition transition-metal catalysis tetrahydrofuran lignans natural products

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Real-time identification of multiple nanoclusters with a protein nanopore in single-cluster level

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Nano Research 2024年第1期17卷 262-269页

作者： Ling Zhang Peilei He Huang Chen Qingda Liu Libo Li Xun Wang Jinghong Li Department of chemistry Center for BioAnalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry&Chemical BiologyTsinghua UniversityBeijing 100084China School of chemistry and Chemical Engineering Guangdong Prov Key Lab Green Chem Prod TechnolSouth China University of TechnologyGuangzhou 510640China New Cornerstone Science Laboratory Shenzhen 518054China Beijing institute of Life Science and Technology Beijing 102206China Center for BioAnalytical chemistry Hefei National Laboratory of Physical Science at MicroscaleUniversity of Science and Technology of ChinaHefei 230026China

It is important and challenging to analyze nanocluster structure with atomic ***,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell time–current blockage spectra and translocation event frequency which sensitively depended on their *** such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be *** nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and ***,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with *** nanopore platform provides a novel powerful tool for nanocluster characterization.

关键词： nanopore single-molecule nanocluster polyoxometalates real-time detection

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

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