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CCS Chemistry 2024年第7期6卷 1662-1671页

作者： Tamara Rodríguez-Prieto Darren Wragg Nicole Heiduk Mihyun Park Nicole Strittmatter Roland A.Fischer Angela Casini Guillermo Moreno-Alcántar Chair of Medicinal and Bioinorganic Chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Professorship for Analytical Chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Chair of inorganic and MetalOrganic Chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Munich Data Science institute(MDSI) Technical University of Munich85748 Garching b.München

The use of three-dimensional self-assembled metallacages(MCgs)as multimodal drug platforms holds great ***,the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still *** this context,this work reports on the integration of a gold(III)porphyrin scaffold into a prismatic MCg structure and explores its application for multimodal therapy of cancer in vitro,namely enabling both photodynamic therapy and *** experimental approaches with a state-of-the-art metadynamics theoretical study,we discovered that the gold cage shows unprecedented host-guest interaction-driven selective stabilization of guanine-quadruplex(G4)structures-validated anticancer drug targets-disclosing a new mechanism to pursue in the design of supramolecular drugs.

关键词： gold metallacages porphyrins G4stabili-zation host-guestchemistry anticanceragents

Unlocking single-atom catalysts via amorphous substrates

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Nano Research 2024年第5期17卷 3533-3546页

作者： Bohua Sun Mingyuan Xu Xiaoxia Li Baohong Zhang Rui Hao Xiaoyu Fan Binbin Jia Dingshun She School of Engineering and Technology China University of Geosciences(Beijing)Beijing 100083China Zhengzhou institute China University of Geosciences(Beijing)Zhengzhou 451283China College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002China School of Chemistry Beihang UniversityBeijing 100191China Chinese Academy of Sciences(CAS)Key Laboratory of Nanosystem and Hierarchy Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China National Engineering Research Center of Nonferrous Metals Materials and Products for New EnergyChina GRINM Group Co.Ltd.Beijing 100088China

Single-atom catalysts(SACs)reveal great potential for application in catalysis due to their fully exposed active *** general,single atoms(SAs)and the coordination substrates need to have strong interactions or charge transfer to ensure the atomic dispersion,which requires the selection of a suitable substrate to stabilize the target *** studies have demonstrated that amorphous materials with abundant defects and coordinatively unsaturated sites can be used as substrates for more efficient capturing SAs,further enhancing the catalytic *** this review,we discuss recent research progress of SAs loaded on amorphous substrates for enhanced catalytic ***,we summarize the commonly used amorphous substrates for stabilizing ***,we present several advanced applications of amorphous SACs in the field of catalysis,including electrocatalysis and *** then,we also clarify the synergistic mechanism between SAs and amorphous substrate on catalytic ***,we summarize the challenges with our personal views and provide a critical outlook on how amorphous SACs continue to evolve.

关键词： single-atoms amorphous substrate synthetic strategy catalysis

Porous organic cages as a novel platform for second harmonic generation

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Science China Chemistry 2024年第11期67卷 3669-3674页

作者： Feng Shui Yunqin Zhang Mao Yi Xiongli Liu Lin Li Shuo Zhang Yongshen Zheng Yongtao Yao Qiao Zhao Baiyan Li Xianhe Bu School of Materials Science and Engineering National Institute for Advanced Materials TKL of Metal and Molecule-Based Material Chemistry Nankai University National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of Technology

Second harmonic generation(SHG) is one of the most extensively applied nonlinear optical phenomena. Compared to traditional inorganic SHG materials, organic SHG materials, including non-centrosymmetric small molecular crystals and organic polymers, have been extensively explored for SHG optics due to their advantageous properties, including high light-induced damage threshold, ultrafast response speed, high polarization ratio, wide transparency range, and elevated dielectric constant. However,in organic SHG materials, most small molecular crystals often show poor thermal stability(<200 °C) due to their low molecular weight, which is an important obstacle for practical application under high temperatures. On the other hand, the difficulty in the growth of large-size crystals as well as the disorderly array of chromospheres on polymer chains associated with organic polymers have hindered their widespread application in SHG due to the requirements of processability and ***, it is significantly necessary to develop novel organic SHG material with high thermal stability, large-size crystals,excellent processability, high homogeneity, and a well SHG effect. In the contribution, we developed herein porous organic cages(POCs) as a novel platform for SHG optics. Thanks to its inherent macromolecular composition and zero-dimensional discrete structures, POCs can not only solve the instability problem of small molecule crystals but also overcome the drawbacks in growing large-size crystals for organic polymer. The obtained two POCs with chiral asymmetric centers(CPOC-R-5 and CPOCS-7) display advantageous features for SHG optics including well SHG performance, large-size crystal(5 mm×3 mm×1 mm),high thermal stability(≥250 °C), wide transparency window(750–2,000 nm) and high polarization ratio(up to 94.5%). This work thus develops POCs as a new platform toward the construction of organic NLO materials with the potential application in sorts of SHG optics.

关键词： porous organic cages second harmonic generation novel SHG platform high thermal stability large-size single crystal

The first chiral cerium halide towards circularly-polarized luminescence in the UV region

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Science China Chemistry 2024年第6期67卷 1961-1968页

作者： Xinyi Niu Zhichao Zeng Zhaoyu Wang Haolin Lu Bing Sun Hao-Li Zhang Yongsheng Chen Yaping Du Guankui Long Tianjin Key Lab for Rare Earth Materials and Applications Renewable Energy Conversion and Storage CenterSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China Tianjin Key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China State Key Laboratory of Applied Organic Chemistry Key Laboratory of Special Function Materials and Structure Design(Ministry of Education)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China The Centre of Nanoscale Science and Technology and State Key Laboratory of Elemento-Organic Chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China

Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting ***,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely *** fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/*** chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and *** emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV ***,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV *** work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral *** RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.

关键词： chiral rare-earth halide ultraviolet circularly-polarized luminescence d-f transition rare-earth halide perovskite chiral perovskite

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Antibody-platinum(IV)prodrugs conjugates for targeted treatment of cutaneous squamous cell carcinoma

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Journal of Pharmaceutical Analysis 2024年第3期14卷 389-400页

作者： Xiangye Yin Yingjie Zhuang Haiqin Song Yujian Xu Fan Zhang Jianxin Cui Lei Zhao Yingjie Yu Qixu Zhang Jun Ye Youbai Chen Yan Han Department of Plastic and Reconstructive Surgery The First Medical CenterChinese PLA General HospitalBeijing100853China Department of General Surgery Ruijin HospitalShanghai Jiao Tong University School of MedicineShanghai200023China State Key Laboratory of Organic-inorganic Composites Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing100029China Department of Plastic Surgery University of Texas MD Anderson Cancer CenterHoustonTX77030USA State Key Laboratory of Bioactive Substance and Function of Natural Medicines Institute of Materia MedicaChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing100050China

Antibody-drug conjugates(ADCs)are a new type of targeting antibodies that conjugate with highly toxic anticancer drugs via chemical linkers to exert high specificity and efficient killing of tumor cells,thereby attracting considerable attention in precise oncology ***(Cet)is a typical antibody that offers the benefits of good targeting and safety for individuals with advanced and inoperable cutaneous squamous cell carcinoma(cSCC);however,its anti-tumor activity is limited to a single ***(CisPt)shows good curative effects;however,its adverse effects and non-tumor-targeting ability are major *** this study,we designed and developed a new ADC based on a new cytotoxic platinum(IV)prodrug(C8Pt(IV))and *** so-called antibody-platinum(IV)prodrugs conjugates,named Cet-C8Pt(IV),showed excellent tumor targeting in ***,it accurately delivered C8Pt(IV)into tumor cells to exert the combined anti-tumor effect of Cet and ***,metabolomic analysis showed that Cet-C8Pt(IV)promoted cellular apoptosis and increased DNA damage in cSCC cells by affecting the vitamin B6 metabolic pathway in tumor cells,thereby further enhancing the tumor-killing ability and providing a new strategy for clinical cancer treatment using antibody-platinum(IV)prodrugs conjugates.

关键词： Antibody drug conjugate Cutaneous squamous cell carcinoma DNA damage Platinum drug Targeted therapy

Reinforced Lewis covalent bond by twinborn nitride heterostructure for lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第1期88卷 363-372,I0009页

作者： Yaochen Song Pengkai Tang Yanjie Wang Yi Wang Linnan Bi Qi Liang Liang He Qingyu Xie Yiyong Zhang Peng Dong Yingjie Zhang Yao Yao Jiaxuan Liao Sizhe Wang Yangtze Delta Region institute(QuZhou) University of Electronic Science and Technology of ChinaQinzhou 324000ZhejiangChina School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina National and Local Joint Engineering Laboratory for Lithium-ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093YunnanChina School of Materials Science and Engineering Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic MaterialsShaanxi University of Science&TechnologyXi’an 710021ShaanxiChina School of Environmental Science and Engineering North China Electric Power UniversityBaoding 071003HebeiChina

The practical application of lithium-sulfur(Li-S)batteries,as promising next-generation batteries,is hindered by their shuttle effect and the slow redox ***,a tungsten and molybdenum nitride heterostructure functionalized with hollow metal-organic framework-derived carbon(W_(2)N/Mo_(2)N)was proposed as the sulfur *** hollow spherical structure provides storage space for sulfur,enhances electrical conductivity,and inhibits volume *** metal atoms in the nitrides bonded with lithium polysulfides(Li PSs)through Lewis covalent bonds,enhancing the high catalytic activity of the nitrides and effectively reducing the energy barrier of Li PSs redox ***,the high intrinsic conductivity of nitrides and the ability of the heterostructure interface to accelerate electron/ion transport improved the Li+*** leveraging the combined properties of strong adsorption and high catalytic activity,the sulfur host effectively inhibited the shuttle effect and accelerated the redox kinetics of Li ***-efficiency Li+transmission,strong adsorption,and the efficient catalytic conversion activities of Li PSs in the heterostructure were experimentally and theoretically *** results indicate that the W_(2)N/Mo_(2)N cathode provides stable,and long-term cycling(over 2000 cycles)at 3 C with a low attenuation rate of 0.0196%per *** design strategy of a twinborn nitride heterostructure thus provides a functionalized solution for advanced Li-S batteries.

关键词： Heterostructure adsorption Redox kinetics

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Comprehension-driven design of advanced multi-block single-ion conducting polymer electrolytes for high-performance lithium-metal batteries

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Journal of Energy Chemistry 2024年第7期94卷 357-359页

作者： Xu Dong Dominic Bresser Helmholtz institute Ulm(HIU) Helmholtzstrasse 1189081 UlmGermany Karlsruhe institute of Technology(KIT) P.O.Box 364076021 KarlsruheGermany

The continuously growing importance of batteries for powering(hybrid)electric vehicles and storing renewable energy has prompted a renewed focus on lithium-metal batteries(LMBs)in recent years,as its high theoretical specific capacity of about 3860 mA h g^(-1) and very low redox potential(-3.04 V *** standard hydrogen electrode)promise substantially higher energy densities compared to current lithium-ion batteries(LIBs)[1].However,lithium metal electrodes face severe challenges associated with the risk of dendritic lithium deposition and the high reactivity with traditional organic liquid electrolytes,resulting in a continuous loss of electrochemically active lithium and a relatively low Coulombic efficiency[2].To address these challenges,solid inorganic and polymer electrolytes have emerged as a potentially saferalternative.

关键词： lithium polymer prompt

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Emerging analytical methods to characterize zeolite-based materials

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National Science Review 2022年第9期9卷 47-66页

作者： Sophie H.van Vreeswijk Bert M.Weckhuysen inorganic Chemistry and Catalysis Debye Institute for NanomaterialsUtrecht University

Zeolites and zeolitic materials are,through their use in numerous conventional and sustainable applications,very important to our daily lives,including to foster the necessary transition to a more circular *** characterization of zeolite-based materials has a tremendous history and a great number of applications and properties of these materials have been discovered in the past *** review focuses on recently developed novel as well as more conventional techniques applied with the aim of better understanding zeolite-based *** explored analytical methods,*** probe tomography,scanning transmission X-ray microscopy,confocal fluorescence microscopy and photo-induced force microscopy,are discussed on their important contributions to the better understanding of zeolites as they mainly focus on the micro-to nanoscale chemical imaging and the revelation of structure-composition-performance *** other techniques have a long and established history,*** magnetic resonance,infrared,neutron scattering,electron microscopy and X-ray diffraction techniques,and have gone through increasing developments allowing the techniques to discover new and important features in zeolite-based *** to the increasing application of these methods,multiple techniques are nowadays used to study zeolites under working conditions(*** in situ/operando mode of analysis) providing new insights in reaction and deactivation mechanisms.

关键词： catalysis zeolites spectroscopy microscopy structure–composition–performance relationships

Liquid metal as an efficient protective layer for lithium metal anodes in all-solid-state batteries

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Carbon Energy 2024年第7期6卷 219-229页

作者： Shiqiang Zhou Mengrui Li Peike Wang Lukuan Cheng Lina Chen Yan Huang Boxuan Cao Suzhu Yu Qingju Liu Jun Wei Shenzhen Key Laboratory of Flexible Printed Electronics Technology Harbin Institute of TechnologyShenzhenChina School of Materials Science and Engineering Harbin Institute of TechnologyShenzhenChina State Key Laboratory of Advanced Welding and Joining Harbin Institute of TechnologyHarbinChina Yunnan Key Laboratory for Micro/Nano Materials and Technology School of Materials and EnergyYunnan UniversityKunmingChina

Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and ***,inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial ***,we report a liquid metal-coated lithium metal(LM@Li)anode strategy to improve the contact between lithium metal and a Li6PS5Cl inorganic *** LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2mA cm^(-2) and a significantly higher critical current density of 9.8 mAcm^(-2) at 25°*** addition,a full battery assembled with a high-capacity composite LiNbO3@-LiNi_(0.7)Co_(0.2)Mn_(0.1)O_(2)(LNO@NCM721)cathode shows stable cycling *** and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.

关键词： all-solid-state batteries interface engineering liquid metals lithium metal anodes

Dynamic in situ reconstruction of NiSe2 promoted by interfacial Ce2（CO3）2O for enhanced water oxidation

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Journal of Energy Chemistry 2024年第11期 472-480页

作者： Fengli Wei Jinghao Shen Jiayin Xie Zuyang Luo Luyan Shi Tayirjan Taylor Isimjan Xiulin Yang Jieshan Qiu Bin Wu Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical Sciences Guangxi Normal University Saudi Arabia Basic Industries Corporation (SABIC) at King Abdullah University of Science and Technology (KAUST) State Key Laboratory of Chemical Resource Engineering State Key Laboratory of Organic-Inorganic Composites College of Chemical Engineering Beijing University of Chemical Technology Helmholtz-Zentrum Berlin für Materialien und Energie GmbH institute of Physics Humboldt University Berlin

Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic ***,we present a synthesis of NiSe2-Ce2（CO3）2O heterostructure and demonstrate the efficacy of interfacial Ce2（CO3）2O in promoting the formation of catalytically active centers to improve oxygen evolution ***-situ Raman spectroscopy shows that incorporation of Ce2（CO3）2O into NiSe2causes a cathodic shift of the Ni2+→Ni3+transition *** electrochemical impedance spectroscopy reveals that strong electronic coupling at heterogeneous interface accelerates charge transfer ***,density functional theory calculations suggest that actual catalytic active species of NiOOH transformed from NiSe2,which is coupled with Ce2（CO3）2O,can optimize electronic structure and decrease the free energy barriers toward fast oxygen evolution reaction（OER） ***,the resultant NiSe2-Ce2（CO3）2O electrode exhibits remarkable electrocatalytic performance with low overpotentials(268/304 mV@50/100 mA cm-2) and excellent stability(50 mA cm-2for 120 h) in the alkaline *** work emphasizes the significance of modulating the dynamic changes in developing efficient electrocatalyst.

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