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Zinc Ion-Induced Immune Responses in Antitumor Immunotherapy

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CCS Chemistry 2024年第9期6卷 2210-2229页

作者： Ying Yang Huanhuan Fan Xinyu Xu Shankun Yao Wenhao Yu Zijian Guo State Key Laboratory of coordination Chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center(ChemBIC)Nanjing UniversityNanjing 210023

Zinc has emerged as a crucial metal in the field of antitumor *** its recognized significance,the specific molecular mechanisms behind zinc ion-mediated antitumor immune responses remain inadequately ***,we present a comprehensive analysis of the effects of zinc ions on immune regulation in antitumor *** ions overload within tumor cells results in the generation of reactive oxygen species(ROS)through two mechanisms:the leakage of electrons from aerobic respiration in mitochondria and the oxidation of reduced nicotinamide adenine dinucleotide phosphate(NADPH)by NADPH oxidase 1(NOX1).The accumulation of ROS and the resulting damage to mitochondrial DNA(mtDNA)activate multiple signaling pathways,leading to the production of high levels of interferons and inflammatory ***,excessive zinc ions induce tumor cell pyroptosis through two pathways:the caspase-1/GSDMD-dependent canonical pathway and the caspase-3/GSDME-dependent alternative pathway,leading to the exposure of many damage-associated molecular patterns(DAMPs).As a result,strong systemic antitumor immunity is triggered,leading to the inhibition of tumor *** study unveils the intricate network of signaling pathways mediated by zinc ions in the tumor microenvironment(TME).Such findings not only lay a solid foundation for the development of zinc-based antitumor drugs but also advance the field of zinc-based metalloimmunotherapy.

关键词： zinc ion immune responses signal transduction pyroptosis antitumor immunotherapy

Construction of N-doped copper metal–organic frameworks for promoting photocatalytic carbon dioxide reduction to ethylene

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Science China Chemistry 2024年

作者： Fan Guo Zong-Zheng He Peng Wang Xiao-Yu Zhang Hongjian Yu Qin-Chao Wang Wei-Yin Sun School of Chemistry and Chemical engineering Yangzhou University coordination Chemistry Institute State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing National Laboratory of Microstructures Collaborative Innovation Center of Advanced Microstructures Nanjing University

engineering nonmetallic atom-doped metal-organic framework （MOF） catalyst to promote C-C coupling and realize conversion of CO2into C2 multi-carbon hydrocarbon products is still ***,with 2-methylimidazole as a dopant of N element,an N-doped NH2-CuBDC catalyst was obtained via a facile and simple stirring *** illumination,compared with catalytic CO2reduction to C1 product of CO by original MOF,N-doped NH2-CuBDC can motivate generation of C2H4,which is difficult to achieve in photocatalytic system by MOF-based *** transfer rates of photo-generated charges have been expedited due to the high electron density around Cu catalytic sites after *** importantly,C–C coupling intermediate CO–CHO*was identified by in situ Fourier transform infrared spectroscopy during the catalytic CO2reduction reaction process,which further indicates the presence of Cu–N sites in the NH2-CuBDC can facilitate the formation of *** work uncovers a new paradigm to design photocatalysts for enhancing the reduction of CO2to C2 products.

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Chiral multiple-resonance thermally activated delayed fluorescence materials based on chiral spiro-axis skeleton for efficient circularly polarized electroluminescence

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Science China Chemistry 2024年第7期67卷 2257-2264页

作者： Shi-Quan Song Xiao Han Zhong-Zhong Huo Ching-Fai Yip Xian-Fang Hong Meng-Ning Ding You-Xuan Zheng State Key Laboratory of coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Key Laboratory of Mesoscopic Chemistry of Ministry of Education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chiral luminescence materials have potential applications in the field of three-dimensional displays due to their circularly polarized luminescence(CPL)***,the further development of circularly polarized organic light-emitting diodes(CP-OLEDs)needs to meet the requirements of high efficiency,high color purity,low cost,and high dissymmetry factor(gPLor gEL),chiral multiple resonance thermally activated delayed fluorescence(MR-TADF)materials are considered as candidates in these ***,based on a pair of chiral spirofluorene precursors,two pairs of high-performance chiral MR-TADF emitters((R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB)are developed,which exhibit strong emissions peaking at 491 and 502 nm in toluene with full-width at half-maximum values of 25 and 33 nm,*** addition,small singlet–triplet energy gaps of 0.15 and 0.10 eV with high absolute photoluminescence efficiencies of 95.0%and 96.7%are observed for p-Spiro-DtBuCzB and m-Spiro-DtBuCzB molecules,*** based on p-Spiro-DtBuCzB and m-Spiro-DtBuCzB display high maximum external quantum efficiencies of 29.6%and 33.8%,*** importantly,CP-OLEDs present symmetric circularly polarized electroluminescence spectra with|gEL|factors of 3.36×10^(-4)and 7.66×10^(-4)for devices based on(R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB enantiomers,respectively.

关键词： chiral spiro-axis skeleton-based material multiple resonance thermally activated delayed fluorescence circularly polarized electroluminescence dissymmetry factor external quantum efficiency

Self-Powered Piezo-Supercapacitors Based on ZnO@Mo-Fe-MnO2 Nanoarrays

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Energy & Environmental Materials 2024年第4期7卷 304-314页

作者： Luo Sun Zhiguo Ye Xinyuan Peng Shaojie Zhuang Duosheng Li Zhong Jin School of Materials Science and engineering Nanchang Hangkong University State Key Laboratory of coordination Chemistry MOE Key Laboratory of Mesoscopic Chemistry MOE Key Laboratory of High Performance Polymer Materials and Technology Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering Nanjing University

The development of self-charging supercapacitor power cells （SCSPCs） has profound implications for smart electronic devices used in different ***,we epitaxially electrodeposited Mo-and Fe-codoped MnO2films on piezoe... 详细信息

关键词： MnO2 piezoelectric self-charging supercapacitors ZnO nanoarray

High-throughput structure determination of polycrystalline functional materials: a platform for automated 3DED/MicroED data collection

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Science China Chemistry 2024年

作者： Zhenghan Zhang Zhengyin Liang Chao Ma Cong Lin Jian Li State Key Laboratory of coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University Department of Mechanical engineering The Hong Kong Polytechnic University

Structure determination plays the most crucial role in the discovery of novel functional materials, because only by knowing the intrinsic structures can we accurately and completely understand their properties and applications. However, most new materials are obtained in polycrystalline form or even as mixtures with multiple phases when first synthesized, presenting significant challenges in their structure determination and phase elucidation. Fortunately, the developed three-dimensional electron diffraction (3DED/MicroED) has provided a promising solution to overcome these challenges. In this study, we have constructed a state-of-the-art 3DED/MicroED data acquisition equipment by integrating a hybrid-pixel detector with a script developed for SerialEM, and thus successfully developed an automated 3DED/MicroED method for the high-throughput structure determination. To demonstrate its effectiveness, a multiphase sample with complex porous structures is employed, showcasing that individual phases and their structures can be identified and determined, respectively. One remarkable finding is the identification of an impurity metal-organic framework (MOF) that is completely invisible to traditional powder X-ray diffraction in a supposedly “pure” commercial MOF sample. Additionally, our method also enables the atomic-resolution structure determination of flexible covalent organic framework materials, which are highly sensitive to electron beams. Moreover, a new microporous aluminoborate is discovered using this rapid structure determination method. These experimental results highlight the enormous potential of our 3DED/MicroED method in the field of new materials discovery, offering a powerful tool for the structure determination of polycrystalline functional materials.

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Metal-organic framework and its composites modulate macrophage polarization in the treatment of inflammatory diseases

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Chinese Chemical Letters 2024年第5期35卷 45-56页

作者： Feifei Wang Hang Yao Xinyue Wu Yijian Tang Yang Bai Hui Chong Huan Pang School of Chemistry and Chemical engineering Yangzhou UniversityYangzhou 225002China School of Pharmacy Changzhou UniversityChangzhou 213164China State Key Laboratory of coordination Chemistry Nanjing UniversityNanjing 210023China

Metal-organic framework(MOF)is a periodic sexual network structure with large surface area and high porosity,which is assembled by inorganic nodes and organic ligands through coordinate covalent *** have the advantages of controllable pore size and shape,large specific surface area,easy modification and more active *** addition,MOF based nanoenzymes display excellent enzyme catalytic activity due to their special structure and multiple exposed metal active sites,controlling the production of reactive oxygen species(ROS)in cells or the body,and thus regulating the polarization of *** article reviews the mechanism of MOF material regulating macrophage polarization and the function of macrophages with different *** utilizing the excellent properties of MOFs and the advantages of combining them with bioactive materials,we have discovered their excellent applications in the treatment of inflammatory ***,we discussed the current challenges and prospects faced by MOF based composite *** expect that the research in this developing field will play a more important role in combating inflammatory diseases in the field of nanomedicine.

关键词： Metal-organic framework Inflammation Macrophage polarization Reactive oxygen species Nanozyme activity

Combining cisplatin and a STING agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： Shuren Zhang Dongfan Song Wenhao Yu Ji Li Xiaoyu Wang Yachao Li Zihan Zhao Qi Xue Jing Zhao Jie P.Li Zijian Guo State Key Laboratory of coordination Chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University Department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of Chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STING) agonists are promising cancer therapeutic regimens because they can amplify STING activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two PtIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STING agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a Pt chemotherapeutic drug and STING agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STING agonist single-molecule multitarget metalloimmunology

MicroED as a powerful technique for the structure determination of complex porous materials

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Chinese Journal of Structural Chemistry 2024年第3期43卷 41-54页

作者： Chao Ma Cong Lin Jian Li State Key Laboratory of coordination Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityKowloonHong Kong China

Porous materials have garnered significant attention in recent *** the intrinsic relationship between their structures and properties requires precise knowledge of their atomic ***-crystal X-ray diffraction(SCXRD)has traditionally been the primary method for elucidating such structures,but it demands large,high-quality crystals,often exceeding 5μm in *** growth of these crystals can be a time-consuming process,especially for one-and two-dimensional *** explore structures at the nanoscale,MicroED(microcrystal electron diffraction(ED))offers unprecedented insights into the realm of *** revolutionary technique enables researchers to uncover intricate details within nanoscale structures,promising to reshape our fundamental understanding of *** this review,we delve into the applications of MicroED in the study of various porous materials,including zeolites,metal-organic frameworks(MOFs),and covalent organic frameworks(COFs).We emphasize the pivotal role of MicroED in nanomaterial characterization,enabling precise crystallographic analysis and phase identification.

关键词： Atomic structure MicroED Porous materials Three-dimensional electron diffraction

Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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Science China Chemistry 2024年第3期67卷 1000-1007页

作者： Kun Wu Pei-Wen Cheng Xin-Yi Liu Ji Zheng Xiao-Wei Zhu Mo Xie Puxin Weng Weigang Lu Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China Guangdong Rare Earth Photofunctional Materials engineering Technology Research Center School of Chemistry and EnvironmentJiaying UniversityMeizhou 514015China

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species(ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers(POPs). Benefiting from the extent of local polarization, the thiophene-containing POP(JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP(JNU-217) and the benzenecontaining POP(JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

关键词： porous organic polymer local polarization photocatalytic aerobic oxidation charge separation reactive oxygen species exciton binding energy