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Single thiolate replacement of metal nanoclusters

Science China Chemistry 2024年第2期67卷 523-528页

作者： Ambreen Ambreen Yue Zhou Wanmiao Gu Qing You Liang Fang Guoqing Bian Nan Yan Nan Xia Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyInstitute of Solid State PhysicsHefei Institutes of Physical Science(HFIPS)Chinese Academy of SciencesHefei230031China University of Science and Technology of China Hefei230601China Institute of Physical Science and Information Technology Anhui UniversityHefei230601China

Surface thiolates play important roles in evincing the structures and properties of thiolated metal nanoclusters—one type of recently emerging inorganic-organic hybrids,and thus the thiolate substitution,especially single thiolate substitution,is highly desirable for subtly tailoring the structures and properties of metal nanoclusters.However,such a single-thiolate substituting is challenging,and its influence on the metal-metal and metal-sulfur bonds remains mysterious due to the absence of the singlethiolate-substituted structure.Here,we developed a combined method,concurrently synthesized the single-thiolate-substituted nanocluster and its parent nanocluster,and successfully resolved their structures by single crystal X-ray crystallography,which reveals that the single thiolate substitute has an obvious influence on the metal-metal and metal-sulfur bond lengths although it has no effect on the absorption profile.Interestingly,the metal-metal and metal-sulfur bonds show various thermal extensibility and even the negative thermal expansion phenomena of the Au–S bond were observed in the single-thiolate-substituted nanocluster.The bond length-related stability was also observed.Overall,this study highlights a novel synthesis method and offers novel structural insights and an in-depth structure-property correlation of thiolated metal nanoclusters.

关键词： metal nanoclusters single thiolate replacement thermal expansion stability intercluster interaction

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Insight into Lithium–sulfur batteries performance enhancement: from metal nanoparticles to metal nanoclusters to single metal atoms

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Tungsten 2024年第3期6卷 504-521页

作者： Shuang Ma Qing-Ling Ruan Xue-Cheng Liu Gui-Jun Zhu Die Yuan Ling-Qiao Hu Yu-Mei Huang Xing-Xing Gu Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and Resources Chongqing Technology and Business University National Research Base of Intelligent Manufacturing Service Chongqing Technology and Business University

Lithium-sulfur(Li-S) batteries have attracted much attention and developed rapidly in recent years due to their high energy density,low cost,and environment-friendly.However,its commercialization process still encounters various obstacles.Among them,the sulfur cathode is easy to dissolve and shuttle,resulting in the loss of active substances and the severe growth of lithium anode dendrites,which is one of the biggest obstacles.Improving the redox conversion kinetics of sulfur cathode is expected to fundamentally alleviate the shuttle phenomenon of poly sulfides.Therefore,this paper reviews the effects of metal nanoparticles to metal nanoclusters to metal single-atom catalysts on improving the redox of Li-S batteries,to let researchers better understand the size effect on the kinetics of sulfur cathodes in Li-S batteries,which will provide important guidance for the future large-scale commercialization of Li-S batteries.

关键词： Lithium–sulfur batteries metal nanoparticles metal nanoclusters metal single atoms Size effects

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The synthesis of fluorescent nanoclusters based on the etching reaction

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Nano Research 2024年第5期17卷 4631-4638页

作者： Hongbin Lin Yitao Cao Qiaofeng Yao Tiankai Chen Huiting Shan Jianping Xie Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)and Key Laboratory of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Key Laboratory of Integrated Organic CircuitsMinistry of EducationDepartment of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Thiolate-protected atomically precise nanoclusters(NCs)demonstrate a series of unique luminescent characteristics attributed to their various peculiar electronic structures.Therefore,fluorescent NCs present extraordinary practical values in biosensing and bioimaging research fields.Nevertheless,restricted by the types of fluorescent NCs,there are great difficulties in promoting the development of NCs in fluorescent research areas.As a result,it is of significant necessity for researchers to develop new synthetic pathways to produce high-quality fluorescent NCs.According to the analysis about the structural characteristics of fluorescent NCs,some general features like longer motif and higher ligand-to-metal ratio can be found,consistent to some presented regularities in etching reaction.Consequently,in this work,we used Au_(25)(MHA)_(18)(MHA=6-mercaptohexanoic acid)as a model nanocluster and utilized the etching reaction to systematically explore etching products and their corresponding luminescent properties.Moreover,we also identified three main reaction processes in the entire etching reaction process,which can generate new metal nanocluster species with various fluorescent properties.Hence,the etching reaction will provide a good platform to produce new luminescent metal NC species.

关键词： etching reaction metal nanoclusters fluorescent properties fluorescent conversion

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Cationic antibacterial metal nanoclusters with traceable capability for fluorescent imaging the nano–bio interactions

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Nano Research 2023年第1期16卷 999-1008页

作者： Yixiao Li Shaohua Qu Yumeng Xue Lianbing Zhang Li Shang School of Materials Science and Engineering Northwestern Polytechnical UniversityXi’an 710072China School of Life Sciences Northwestern Polytechnical UniversityXi’an 710072China Northwestern Polytechnical University Chongqing Technology Innovation Center Chongqing 400000China

A thorough understanding of antimicrobial mechanism is of great importance for developing novel,efficient antibacterial agents.While cationic nanoparticles,such as metal nanoclusters(NCs),represent an attractive type of antibacterial nanoagents,their interactions with bacteria remains largely un-elucidated.Herein,we report the synthesis of cationic bovine serum albuminprotected AuAgNCs(cBSA-AuAgNCs),which exhibit both near-infrared(NIR)fluorescence properties and significant antimicrobial effects.With E.coli and S.aureus as the representative bacteria,we investigated the antimicrobial process of cBSAAuAgNCs in real-time based on their intrinsic fluorescence properties via fluorescence imaging.Our results showed that these cBSA-AuAgNCs exert their antimicrobial effects primarily by attaching on the outer membrane of bacteria without obvious internalization,which is significantly different from the antibacterial process of negatively-charged metal NCs.Further mechanistic investigation showed that these cationic NCs will cause serious disruption to the bacterial membrane due to strong electrostatic interactions,which then leads to over accumulation of reactive oxygen species(ROS)that finally causes the bactericidal action.This study demonstrates the great potential of cationic luminescent metal NCs as novel,traceable antimicrobial agents,which also provides new tools for further understanding microbial interactions of nanomedicines.

关键词： metal nanoclusters antimicrobial agents bacterial imaging near-infrared fluorescence

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Peptide or Protein-Protected metal nanoclusters for Therapeutic Application

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Chinese Journal of Chemistry 2022年第2期40卷 267-274页

作者： Xiaolei Chen Xiaojun Ren Xueyun Gao Department of Chemistry and Biology Faculty of Environment and Life ScienceBeijing University of TechnologyBeijing 100124China

What is the most favorite and original chemistry developed in your research group?The most favorite and original work we have done is the development of gold nano clusters for diagnostic and therapeutic application.How do you get into this specific field?Could you please share some experiences with our readers?I have a great passion for research on bioanalytical imaging and the biomedical effects of nanomaterials,which may contribute to early diagnosis and treatment of diseases.My research is focused on exploring the mechanism of protein or peptide-protected metal nanoclusters in disease diagnosis and treatment with the expectation of leading to superior therapeutic outcomes.

关键词： metal nanoclusters Biocompatibility Peptides Cell apoptosis Therapeutic mechanism

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Synergistic integration of metal nanoclusters and biomolecules as hybrid systems for therapeutic applications

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Acta Pharmaceutica Sinica B 2021年第5期11卷 1175-1199页

作者： Peng Gao Xin Chang Dagan Zhang Yafei Cai Gen Chen Hao Wang Tianfu Wang Guangdong Key Laboratory of Biomedical Measurements and Ultrasound Imaging Department of Biomedical EngineeringShenzhen UniversityShenzhen 518060China State Key Laboratory of Bioelectronics School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Key Laboratory of Biomedicine in Gene Diseases and Health of Anhui Higher Education Institutes College of Life SciencesAnhui Normal UniversityWuhu 241000China College of Animal Science and Technology Nanjing Agricultural UniversityNanjing 210095China School of Materials Science and Engineering Central South UniversityChangsha 410083China College of Energy Soochow Institute for Energy and Materials Innovationsand Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006China

Therapeutic nanoparticles are designed to enhance efficacy,real-time monitoring,targeting accuracy,biocompatibility,biodegradability,safety,and the synergy of diagnosis and treatment of diseases by leveraging the unique physicochemical and biological properties of well-developed bio-nanomaterials.Recently,bio-inspired metal nanoclusters(NCs)consisting of several to roughly dozens of atoms(metallic composition,and extensive surface bio-functionalization.Hybrid coreeshell nanostructures that effectively incorporate unique fluorescent inorganic moieties with various biomolecules,such as proteins(enzymes,antigens,and antibodies),DNA,and specific cells,create fluorescently visualized molecular nanoparticle.The resultant nanoparticles possess combinatorial properties and synergistic efficacy,such as simplicity,active bio-responsiveness,improved applicability,and low cost,for combination therapy,such as accurate targeting,bioimaging,and enhanced therapeutic and biocatalytic effects.In contrast to larger nanoparticles,bio-inspired metal NCs allow rapid renal clearance and better pharmacokinetics in biological systems.Notably,advances in nanoscience,interfacial chemistry,and biotechnologies have further spurred researchers to explore bio-inspired metal NCs for therapeutic purposes.The current review presents a comprehensive and timely overview of various metal NCs for various therapeutic applications,with a special emphasis on the design rationale behind the use of biomolecules/cells as the main scaffolds.In the different hybrid platform,we summarize the current challenges and emerging perspectives,which are expected to offer in-depth insight into the rational design of bio-inspired metal NCs for personalized treatment and clinical translation.

关键词： metal nanoclusters Biomolecule Nanoparticles Hybrid system Synergistic properties Fluorescence Bioprobe Therapy

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Emerging applications of near-infrared fluorescent metal nanoclusters for biological imaging

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Chinese Chemical Letters 2018年第10期29卷 1436-1444页

作者： Jie Xu Li Shang State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene (NPU) NPU-QMUL Joint Research Institute of Advanced Materials and Structures (JRI-AMAS) Northwestern Polytechnical University

Fluorescent metal nanoclusters（MNCs） have recently emerged as a novel kind of promising fluorescent probes for biological imaging because of their ultrasmall core size（〈2 nm）, strong photoluminescence,facile availability and good biocompatibility. In this review, we provide an update on recent advances in the development of near infrared（NIR）-emitting MNCs in terms of synthesis strategies and bioimaging applications. We mainly focus on the utilization of NIR-emitting MNCs（including Au, Ag, Cu and alloy NCs） either as single modal imaging（fluorescence intensity-based imaging, fluorescence lifetime imaging, two-photon imaging） probes or as multimodal imaging（such as NIR fluorescence/X-ray computed tomography/magnetic resonance imaging, NIR fluorescence/photoacoustic imaging/magnetic resonance imaging, NIR fluorescence/single photon emission computed tomography） probes in biological cells and tissues. Finally, we give a brief outlook on the future challenges and prospects of developing NIR-emitting MNCs for bioimaging.

关键词： metal nanoclusters Fluorescent probes Cellular imaging In vivo Near-infrared

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Ligand Engineering in metal nanoclusters: from Structural Control to Functional Modulation

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Chinese Journal of Structural Chemistry 2020年第7期39卷 1194-1200页

作者： GUAN Zong-Jie WANG Quan-Ming Department of Chemistry Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of EducationTsinghua UniversityBeijing 100084China

Ligand-protected metal nanoclusters have drawn increasing research interest because of their unique physicochemical properties and practical applications.Great efforts have been made in pursuing rational synthesis of metal nanoclusters and establishing the structure-property relationships.As an indispensable part of ligand-protected metal nanoclusters,ligands play multiple roles in determining their structures and properties.In this perspective,we demonstrate the importance of ligand engineering in terms of the control of structures,optical and catalytic properties of metal nanoclusters.Furthermore,we will show that ligand engineering is prospective in structural design and preorganization of surface metal sites.

关键词： metal nanoclusters physicochemical properties structure-property relationship ligand engineering

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Luminescent metal nanoclusters:Biosensing strategies and bioimaging applications

聚集体(英文)

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聚集体(英文) 2021年第1期2卷 114-132页

作者： Yan Xiao ZhennanWu Qiaofeng Yao Jianping Xie Department of Chemical and Biomolecular Engineering National University of Singapore4 Engineering Drive 4SingaporeSingapore College of Chemistry and Chemical Engineering Hubei UniversityWuhanHubeiChina Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Binhai New CityFuzhouChina

metal nanoclusters(MNCs)are ultrasmall metal-organic aggregates,composed of a metal core less than 2 nm and a protecting shell of metal-organic ligand motifs.The controlled aggregation of metal atoms(in the cluster core)and metal-organic ligand motifs(around the cluster core)renders MNCs with numerous molecule-like properties,among which strong and bright luminescence has attracted extensive basic and applied interests.It has now known that aggregation-induced emission is a feasible mechanism for controlling luminescence of MNCs,which makes it particularly useful in biosensing and bioimaging applications.Although the luminescence fundamentals and design principles largely determine the practicality and effectiveness of MNCs in biosensing and bioimaging applications,a systematic summary of this topic is lacking in the current literature.In this review,we aim to provide a concise discussion of the latest developments in biosensing and bioimaging applications of luminescent MNCs,highlighting their luminescence mechanisms,biosensing principles,and bioimaging strategies.Specifically,we first introduce the recent advances in the synthetic chemistry of MNCs,and then briefly discuss the luminescence fundamentals ofMNCs.Then the design strategy and practicality of luminescent MNCs in biosensing and bioimaging applications are exemplified.We conclude the review with our perspectives on the further development of MNC-based optical probes in biosensing and bioimaging applications.Our review is expected to provide guidance for the future practice of designing and synthesizing luminescent MNCs for biomedical and other applications.

关键词： aggregation-induced emission bioimaging biosensor luminescence metal nanoclusters

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Orange-emitting bimetallic nanoclusters combined with cyan-emitting Fe@TAOH as white light-emitting materials

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Chinese Chemical Letters 2022年第1期33卷 298-303页

作者： Wenying Mi Na Shao College of Chemistry Beijing Normal UniversityBeijing 100875China

White-light-emitting diodes(WLEDs)possess many merits,such as high efficiency and stability.Developing cost-effective,environmentally friendly,high-performance luminophores to achieve high-quality,full-spectrum,white lighting is of great importance to the construction and progress of WLEDs.In this work,solid-state,highly luminescent orange-emitting nanoclusters(MgCl_(2)-Lys-Ag/Au NCs)were prepared via the salt-induced precipitation of Lys-Ag/Au NCs from solution,which showed a high absolute quantum yield of 44.5%.A cyan-emitting metal-organic framework(MOF)-like nanomaterial(named Fe@TAOH)was also prepared by the self-assembly of the coordination compound of Fe^(3+)and TAOH acted upon by H_(3)PO_(4) via H-bonding andπ-πstacking interactions,which showed an emission peak at 485 nm and an absolute quantum yield of 21.7%.The potential application of the two facile-synthesis,low toxicity,and highly luminescent materials in WLEDs was investigated.The WLEDs was constructed by coating powdered Fe@TAOH and MgCl_(2)-Lys-Ag/Au NCs samples on commercial GaN LED chip with 365 nm emissions,and it exhibited acceptable white light characteristics with a CIE color coordinates and a color rendering index(CRI)of(0.28,0.34)and 79.6,respectively,implying good prospects in the field of WLEDs.

关键词： metal nanoclusters Salt-mediated precipitation Fe@TAOH MOFs Self-assembly White light-emitting materials

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