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Application of mannose-modified fullerene immunomodulator selectively polarizes tumor-associated macrophages potentiating antitumor immunity

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Nano Research 2023年第11期16卷 12855-12863页

作者： Haoyu wang Lei Li Xinran Cao Mingming Zhen chunru wang Chunli Bai Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyCAS Research/Education Center for Excellence in Molecular SciencesInstitution Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Polarization of tumor associated macrophages(TAMs)has been a promising therapeutic paradigm for ***,how to achieve precise regulation of TAMs and high efficiency of tumor immunotherapy is still a huge ***,we report dicarboxy fullerene modified with mannose(DCFM)as an immunomodulator to selectively polarize TAMs and prominently boost anti-tumor *** dicarboxy fullerene molecule was synthesized through the Prato reaction and further covalently bonded with mannose,obtaining the DCFM with well-defined *** to the exist of mannose in DCFM,it could accurately recognize mannose receptor in *** cellular experiment results showed that mannose modification could notably promote the uptake of DCFM by the immunosuppressive M2-type macrophages that effectively reprogrammed M2-type macrophages into anti-tumor M1-type macrophages,leading to enhance the phagocytosis of tumor cells by macrophages and inhibiting tumor cells ***,we observed that DCFM could significantly distribute into tumor tissues by in vivo fluorescence ***,DCFM exhibited a superior anti-tumor efficiency in the subcutaneous colorectal tumor *** addition,it showed that DCFM precisely polarized TAMs into M1-type macrophages and actively increased the infiltration of cytotoxic T lymphocytes(CTLs),inducing profound tumor growth inhibition.

关键词： fullerene mannose macrophage targeting tumor-associated macrophage polarization cancer immunotherapy

Covalently bonded two spin centers of paramagnetic metallofullerene dimer

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Nano Research 2021年第12期14卷 4658-4663页

作者： Haibing Meng Yongqiang Chai Chong Zhao Mingzhe Nie chunru wang Taishan wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesZhongguancun North First Street 2Beijing100190China

Paramagnetic endohedral metallofullerenes with well protected unpaired spin have potential applications in molecular-scale qubit processing and magnetoreception system. In this study, a paramagnetic metallofullerene Sc_(3)C_(2)@C_(80) dimer with covalently bonded two spin centers was synthesized. Electron paramagnetic resonance (EPR) results further revealed the varied spin-nuclei couplings and paramagnetic property for Sc_(3)C_(2)@C_(80) dimer. Briefly, the Sc_(3)C_(2)@C_(80) dimer in toluene solution shows EPR hyperfine splittings originating from the spin-Sc couplings. However, the Sc_(3)C_(2)@C_(80) dimer in solid state shows the disappearance of hyperfine structure and a single EPR signal caused by its two-spin-center structure. The transformation of EPR signals can be further finely modulated by controlling the dynamic motion of Sc_(3)C_(2)@C80 dimer in chloronaphthalene. The Sc_(3)C_(2)@C_(80) dimer with two spin centers possesses varied paramagnetic properties, demonstrating its potential as new magnetic material.

关键词： metallofullerene dimer electron spin hyperfine couplings paramagnetic property

Zirconium nitride as a highly efficient nitrogen source to synthesize the metal nitride clusterfullerenes

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Science China Chemistry 2021年第1期64卷 29-33页

作者： Yuxi Lu Jie Zhang Chong Zhao Mingzhe Nie chunru wang Taishan wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotecnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Metal nitride clusterfullerenes(NCFs)have significant applications in molecular electronics,biomedical imaging,and nonlinear optical devices due to their unique ***,their wide applications are limited by the production *** this work,the yields of metal nitride clusterfullerenes M3N@C80(M=Y,Sc,Gd)were greatly enhanced by utilizing zirconium nitride(Zr N)as an efficient nitrogen source for the arc-discharge *** with the traditional synthetic route using N2gas as nitrogen source,the Zr N inside graphite tube can be vaporized simultaneously with metal and graphite,and then afford the high concentration of nitrogen atoms in the arc region,which will promote the formation of metal nitride clusterfullerenes *** Zr N can promote the yields of Y3N@C80,Sc3N@C80and Gd3N@C80,revealing the universal applicability of Zr N as a highly efficient nitrogen ***,the yield of Sc3N@C80was greatly improved when adding Zr N,and it shows over double yield compared to traditional synthetic route using *** addition,Zr N can also enhance the yields of paramagnetic azametallofullerene M2@C79N due to the high concentration of nitrogen atoms in the arc *** new method enhances the production quantity of metal nitride clusterfullerenes and azametallofullerenes,and it will greatly promote the research and application of these molecular carbon materials.

关键词： metal nitride clusterfullerenes zirconium nitride nitrogen source high yield arc-discharge method

Self-assembled array of rectangular single-crystal microtubes of perchlorinated copper phthalocyanines

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Progress in Natural Science:Materials International 2013年第6期23卷 543-548页

作者： Dongwei Yan Yitao Feng chunru wang Advance Technology & Materials Co. Ltd.China Iron&Steel Research Institute Group Beijing National Laboratory for Molecular Sciences Institute of ChemistryChinese Academy of Sciences

The rectangular microtubes array of perchlorinated copper phthalocyanines(G;CuPc),were synthesized by physical vapor deposition technique without using any template or *** synthesis process of the tubular structure is very simple,easy to control,and a little raw material is *** morphology and crystal structure of the obtained samples were analyzed by means of scanning and transmission electron microscopy（SEM and TEM）,X-ray diffraction（XRD）,Fourier transform infrared spectroscopy（FT-IR） and X-ray photoelectron spectroscopy（XPS）.The microtubes have an entire hollow interior,open ends with rectangular cross-section,a large interior of 1.4-1.8 urn width,and the thin walls of 80-100 *** obtained products exhibit excellent crystalline nature,high chemical and thermodynamic stability,excellent biocompatibility,as well as *** is believed that these well-defined microtubular structures of an organic material will be used as active materials for solar cells,nanodevices for field emission apparatus,microchannels for biochip and microvessel for drug delivery.

关键词： Perchlorinated copper phthalocyanines Rectangular microtubes Single-crystal self-assembly Nanodevices Microchannels

Synergistic modulation of spin and fluorescence signals in a nano-Saturn assembled by a metallofullerene and cycloparaphenylene nanohoop

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Nano Research 2023年第2期16卷 3372-3378页

作者： Jie Zhang Zhenlin Qiu Chong Zhao Yuxi Lu wang Li Linshan Liu chunru wang Yuanzhi Tan Taishan wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China University of Chinese Academy of Sciences Beijing 100049China School of Pharmacy Guizhou Medical UniversityGuiyang 550025China

Spin-based interdisciplinary research has attracted considerable attention,and various applications in magnetic memory,quantum science,and precision measuring technology have been *** this study,we induced a fluorescence property in a spin-active molecule by supramolecular assembly and realized a synergistic modulation of its spin and fluorescence properties.A Saturn-shaped supramolecular complex was synthesized using a spin-active metallofullerene Sc_(3)C_(2)@C80 with a fluorescent nanohoop of tetra-benzothiadiazole-based[12]cycloparaphenylene(TB[12]CPP),and its spin and fluorescence properties were comprehensively ***-dependent electron paramagnetic resonance(EPR)spectroscopy and fluorescence analyses were *** changes in the EPR signals and fluorescence peaks were discovered in the temperature range of 170–290 *** on nuclear magnetic resonance observations and theoretical calculations,a temperature-dependent host–guest interaction between Sc_(3)C_(2)@C_(80)and a nanohoop was demonstrated,which explained the synchronous changes in the EPR signals and fluorescence peaks for Sc_(3)C_(2)@C_(80)⊂TB[12]*** application of Sc_(3)C_(2)@C_(80)as a molecular spin system to probe the host–guest interaction was also *** results show that the supramolecular assembly can be used to design advanced spin systems coupled with optical and magnetic behaviors based on paramagnetic and luminescent molecules.

关键词： metallofullerene nanohoop electron spin fluorescence host–guest interaction

A molecular brake hoop for the motion of metal atoms inside fullerene cage

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Science China Chemistry 2022年第8期65卷 1601-1606页

作者： Yuxi Lu Chong Zhao Jie Zhang wang Li Jiayi Liang Linshan Liu Yongguang Li chunru wang Taishan wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China School of Pharmacy Guizhou Medical UniversityGuian New District 550025China College of Material Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China

Molecular machines have attracted extensive attention due to their fancy concept and their potential to influence the science and *** dynamic motion of encapsulated metallic clusters is a distinctive character for endohedral *** the development of molecular rotors based on metallofullerenes,the most challenging issue is how to control the motion of untouchable metallic cluster inside fullerene *** this work,we report a molecular brake hoop for the motion of metal atoms inside fullerene cage.A cycloparaphenylene of[12]CPP was employed to hoop the metallofullerene and produce two supramolecular complexes of Sc_(3)N@C_(80)⊂[12]CPP and Sc_(2)C_(2)@C_(82)⊂[12]***,the temperature-dependent ^(45)Sc nuclear magnetic resonance spectroscopy(NMR)was employed to detect the motion of internal Sc_(3)N and Sc_(2)C_(2) clusters.^(45)Sc NMR results reveal that the[12]CPP can slow down the rotation of internal metallic cluster through host-guest interaction,and thus the[12]CPP can be considered as a molecular brake hoop for the internal metal motion of ***,by means of this molecular brake hoop,the motion of metal atoms inside fullerene cage have expanded range of *** addition,theoretical calculations on Sc_(3)N@C_(80)⊂[12]CPP were executed to illustrate the molecular orientation as well as internal Sc_(3)N *** study would promote the research of endohedral metallofullerene as a molecular rotor.

关键词： metallofullerene molecular rotor molecular brake supramolecular complex dynamic motion

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Luminescent single-molecule magnet of metallofullerene DyErScN@Ih-C80

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Nano Research 2019年第7期12卷 1727-1731页

作者： Mingzhe Nie Jin Xiong Chong Zhao Haibing Meng Kun Zhang Yibo Han Jie Li Bingwu wang Lai Feng chunru wang Taishan wang Beijing National Laboratory for Molecular Sciences Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Beijing National Laboratory of Molecular Science College of Chemistry and Molecular Engineering State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPeking UniversityBeijing 100871China Soochow Institute for Energy and Materials Innovations (SIEMIS) College of PhysicsOptoelectronics and Energy & Jiangsu Key Laboratory of Advanced Carbon Materials and Wearable Energy TechnologiesSoochow UniversitySuzhou 215006China Wuhan National High Magnetic Field Center and School of Physics Huazhong University of Science and TechnologyWuhan 430074China University of Chinese Academy of Sciences Beijing 100049China

Magneto-luminescent molecules have significant applications in data storage and quantum ***,design of these bi-functional molecules coupled with magnetic behavior and photoluminescence is still *** this work,we report a metallofullerene DyErScN @In-C80 exhibiting single-molecule magnet (SMM) behavior and near-infrared *** DyErScN @Ih-C80,two functional lanthanide metal ions of Dy^3+(SMM function) and Er^3+(luminescent function) are integrated inside a fullerene cage using a trimetallic nitride template,and its structure has been unambiguously characterized by single-crystal X-ray *** measurements revealed that DyErScN @Ih-C80 behaves as a SMM with a blocking temperature up to 9 K resulting from the intramolecular magnetic interaction between Dy^3+ and Er^3+ ***,DyErScN @In-C80 exhibits temperature-dependent near-infrared emission around 1.5 pm with multiple splitting peaks from Er^3+,which arises from the influence of Dy^3+ *** study provides a new strategy to synthesize new magneto-luminescent molecule materials.

关键词： metallofullerene single-molecule magnet near-infrared photoluminescence

Oxidization-induced structural optimization of Ni_(3)Fe-N-C derived from 3D covalent organic framework for high-efficiency and durable oxygen evolution reaction

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Nano Research 2023年第5期16卷 6710-6720页

作者： Haibing Meng Bin Wu Tianxiao Sun Long Wei Yunlong Zhang Bo Liu Kai Chen Zhen-Bo wang Shuhui Sun chunru wang Xian-Ming Zhang College of Chemistry Taiyuan University of TechnologyTaiyuan 030024China Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Straße 15Berlin 12489Germany Institute of Physics Humboldt University BerlinNewton-Straße 15Berlin 12489Germany National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China Institute National de La Recherche Scientifique(INRS)-CentreÉnergie Matériaux Télécommunications VarennesQC J3X 1P7Canada Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

NiFe composites have been regarded as promising candidates to replace commercial noble-based electrocatalysts for the oxygen evolution reaction(OER).However,their practical applications still suffer from poor conductivity,limited activity,*** address these issues,herein,by utilizing three-dimensional covalent organic framework(3D-COF)with porous confined structures and abundant coordinate N sites as the precursor,the partially oxidized Ni_(3)Fe nanoalloys wrapped by Ndoped carbon(N-C)layers are constructed via simple pyrolysis and subsequent *** from the 3D curved hierarchical structure,high-conductivity of Ni_(3)Fe and N-C layers,well-distributed active sites,the as-synthesized O-Ni_(3)Fe-NC catalyst demonstrates excellent activity and durability for catalyzing *** and theoretical analyses disclose that both high-temperature oxidization and the OER process greatly promote the formation and exposure of the Ni(Fe)OOH active species as well as lower charge transfer resistance,inducing its optimized OER *** robust graphitized N-C layers with superior conductivity and their couplings with oxidized Ni_(3)Fe nanoalloys are beneficial for stabilizing catalytic centers,thereby imparting O-Ni_(3)Fe-N-C with such outstanding *** work not only provides a rational guidance for enriching and stabilizing high-activity catalytic sites towards OER but also offers more insights into the structural evolution of NiFe-based OER catalysts.

关键词： three-dimensional covalent organic framework(3D-COF) Ni_(3)Fe graphitized N-C layer structure optimization durability

Modulating morphology via side-chain engineering of fused ring electron acceptors for high performance organic solar cells

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Science China Chemistry 2019年第6期62卷 790-796页

作者： Fuwen Zhao Dan He Jingming Xin Shuixing Dai Han Xue Li Jiang Zhixiang Wei Wei Ma Xiaowei Zhan Yongfang Li chunru wang Institute of Chemistry Chinese Academy of Sciences State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Department of Materials Science and Engineering College of Engineering Peking University National Center for Nanoscience and Technology

In this work, four fused ring electron acceptors(FREAs), 2F-C5, 2F-C6, 2F-C8 and 2F-C10, are developed to investigate the effect of side-chain size on the molecular properties and photovoltaic performance of FREA systematically. The elongation of side-chains in the FREAs not only improves their solubility in the processing solvent, but also enhances their miscibility with the donor PBDB-T. It helps the FREA diffuse into the donor PBDB-T during film-formation, thus leading to the decrease in domain size and domain purity from PBDB-T:2F-C5 to PBDB-T:2F-C10 blend films in sequence. The smaller domain size affords more D/A interfaces to benefit exciton dissociation and inhibit monomolecular recombination. However, severe bimolecular recombination occurs when the domain purity decreases to a critical point. Due to the dual function of the increment of side-chain length, both short-circuit current density(J_(SC)) and fill factor(FF) of devices exhibit an evolution of first increasing then decreasing from 2F-C5, 2F-C6, 2F-C8 to 2F-C10 based OSCs. The PBDB-T:2F-C8 based OSCs get a fine balance in morphology with moderate domain size as well as high domain purity simultaneously for the least charge carrier recombination, thus achieving the highest power conversion efficiency of 12.28% with the best J_(SC)(21.27 mA cm^(-2)) and FF(71.96%).

关键词： solar cells fused ring electron acceptor side-chain length morphology