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Aggregate 2024年第1期5卷 345-352页

作者： Bing Yin Lirong Jiang Xiaojian Wang Ying Liu Kaiyang Kuang Mengmeng Jing Chunmin Fang Chuanjun Zhou Shuang Chen Manzhou Zhu Institutes of Physical Science and Information Technology and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationDepartment of Chemistry and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefeiChina

Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic effect.Pt^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,respectively.In the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA concentration.Potential-resolved ECL spectra reveal two ECL emission bands in the presence of TPrA.The ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid state.The ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon electrode.The electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without nanoclusters.Based on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are proposed.These findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.

关键词： AIECLE AIEE electrochemiluminescence nanocluster photoluminescence structure

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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 precision.Herein,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 structures.nanoclusters such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be discriminated.This nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and quantitatively.Furthermore,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with experiments.The nanopore platform provides a novel powerful tool for nanocluster characterization.

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

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Cage-confinement synthesis of MoC nanoclusers as efficient sulfiphilic and lithiophilic regulator for superior Li–S batteries

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Rare Metals 2024年第2期43卷 624-634页

作者： Xing-Yuan Zhang Mei-Na Lei Shan Tian Jian-Gan Wang 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)Xi’an710072China

High-energy-density Li-S batteries are subjected to serious sulfur deactivation and short cycle lifetime caused by undesirable polysulfide shuttle effect and frantic lithium dendrite formation.In this work,a controllable cage-confinement strategy to fabricate molybdenum carbide(MoC)nanoclusters as a high-efficient sulfiphilic and lithiophilic regulator to mitigate the formidable issues of Li-S batteries is demonstrated.The sub-2 nm MoC nanoclusters not only guarantee robust chemisorption and fast electrocatalytic conversion of polysulfides to enhance the sulfur electrochemistry,but also homogenize Li^(+) flux to suppress the lithium dendrite growth.As a consequence,the MoC-modified separator endows the batteries with boosted reaction kinetics,promoted sulfur utilization,and improved cycling stability.A reversible capacity of 701 mAh·g^(−1) at a high rate of 5.0C and a small decay rate of 0.076%per cycle at 1.0C over 600 cycles are achieved.This study offers a rational route for design and synthesis of bifunctional nanoclusers with both sulfiphilicity and lithiophilicity for high-performance Li-S batteries.

关键词： Li-S batteries nanocluster Electrocatalyst Polysulfide shuttle Li dendrites

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Precisely manipulation of core composition of core-shell-type cobalt polyoxoniobates and proton conduction study

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Chinese Chemical Letters 2024年第1期35卷 510-513页

作者： Zheng-Wei Guo Yi Chen Zhe-Hong Chen Xin-Xiong Li Shou-Tian Zheng State Key Laboratory of Photocatalysis on Energy and Environment School of ChemistryFuzhou UniversityFuzhou 350108China

The development of core-shell nanoclusters with controllable composition is of utmost importance as the material properties depend on their constituent elements.However,precisely tuning their compositions at the atomic scale is not easily achieved because of the difficulty of using limited macroscopic synthetic methods for atomic-level modulation.In this work,we report an interesting example of precisely regulating the core composition of an inorganic core-shell-type cobalt polyoxoniobate[Co_(26)Nb_(36)O_(140)]^(32−)by controlling reaction conditions,in which the inner Co-core composition could be tune while retaining the outer Nb-shell composition of resulting product,leading to a series of isostructural species with a general formula of{Co_(26-n)Nb_(36+n)O_(140)}(n=0–2).These rare species not only can display good powder and single-crystal proton conductivities,but also might provide helpful and atomic-level insights into the syntheses,structures and composition modifications of inorganic amorphous core-shell heterometal oxide nanoparticles.

关键词： Polyoxoniobate Core-shell nanocluster Atomic-level modulation Proton conduction

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DNA-silver nanocluster Binary Probes for Ratiometric Fluorescent Detection of HPV-related DNA

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Chemical Research in Chinese Universities 2019年第4期35卷 581-585页

作者： YUAN Yan LI Shaoyuan LUO Lei WANG Qing FANG Hongmei HUANG Jin LIU Jianbo YANG Xiaohai WANG Kemin State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Key Laboratory for Bio-nanotechnology and Molecular Engineering of Hunan Province Hunan University Changsha 410082 P. R. China

Herein, we described a ratiometric strategy based on "chameleon" DNA-silver nanoclusters( DNA-AgNCs) fluorescent binary probes. The strategy was applied to detect high-risk human papillomavirus( HPV) DNA sequences, HPV-16. First, DNA-AgNCs were synthesized by a simple reduction method. The obtained nanoprobes showed typical yellow and red fluorescence of AgNCs. Upon the addition of HPV-16 DNA, the yellow fluorescence of AgNCs was reduced greatly, whereas tlie red fluorescence of AgNCs was increased. The concentration of HPV-16 DNA in the samples was characterized by the ratio of fluorescence intensity at 570 and 630 nm. Tlie ratiometric nanoprobes showed good selectivity for HPV-16 DNA, and the detection limit was 2 ninol/L. In addition, the practical applicability of this strategy was demonstrated by analysing the HPV-16 DNA in hiunan serum, illustrating its potential promise for clinical diagnosis.

关键词： DNA-silver nanocluster Ratiometric Binary probe Human papillomavinis

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Atomically precise metal chalcogenide supertetrahedral clusters:frameworks to molecules,and structure to function

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National Science Review 2022年第1期9卷 128-143页

作者： Jiaxu Zhang Pingyun Feng Xianhui Bu Tao Wu College of Chemistry Chemical Engineering and Material Science Soochow University Department of Chemistry University of California College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University Department of Chemistry and Biochemistry California State University

Metal chalcogenide supertetrahedral clusters(MCSCs) are of significance for developing crystalline porous framework materials and atomically precise cluster chemistry.Early research interest focused on the synthetic and structural chemistry of MCSC-based porous semiconductor materials with different cluster sizes/compositions and their applications in adsorption-based separation and optoelectronics.More recently,focus has shifted to the cluster chemistry of MCSCs to establish atomically precise structure-composition-property relationships,which are critical for regulating the properties and expanding the applications of MCSCs.Importantly,MCSCs are similar to Ⅱ-Ⅵ or Ⅰ-Ⅲ-Ⅵ semiconductor nanocrystals(also called quantum dots,QDs) but avoid their inherent size polydispersity and structural ambiguity.Thus,discrete MCSCs,especially those that are solution-processable,could provide models for understanding various issues that cannot be easily clarified using QDs.This review covers three decades of efforts on MCSCs,including advancements in MCSC-based open frameworks(reticular chemistry),the precise structure-property relationships of MCSCs(cluster chemistry),and the functionalization and applications of MCSC-based micro crystals.An outlook on remaining problems to be solved and future trends is also presented.

关键词： metal chalcogenide nanocluster open framework semiconductor reticular chemistry atomically precise nanochemistry

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Design of platinum single-atom doped metal nanoclusters as efficient oxygen reduction electrocatalysts by coupling electronic descriptor

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Nano Research 2022年第8期15卷 7016-7025页

作者： Qing Liu Xiaoxu Wang Lu Li Keke Song Ping Qian Yuan Ping Feng Beijing Advanced Innovation Center for Materials Genome Engineering University of Science and Technology BeijingBeijing 100083China Department of Physics Faculty of ScienceNational University of SingaporeSingapore 117551Singapore DP Technology Beijing 100080China

Inspired by the single-atom catalysts(SACs)concept,we rationally design a series of Pt single atom catalysts embedded in different transition metal nanoclusters through first-principles calculations.In these so-called“crown-jewel”(CJ)structures,Pt atoms(jewels)occupy the vertex sites of the metal nanocluster(crown)surface.We investigated the thermal stability and oxygen reduction reaction(ORR)catalytic activity of these catalysts.The results reveal that CJ-structured PtCu nanoclusters are stable and possess a comparable or even better ORR activity compared to Pt catalyst,making it a promising candidate for low-cost ORR catalysts.The effect of cluster size on the adsorption strength of ORR intermediates and catalytic property has also been studied.Furthermore,the overall ORR catalytic activity trend of these SACs is explained based on analysis of their electronic properties.A descriptorΨwas established to provide further insight into the correlation between the electronic structure and catalytic activity,which provides a design strategy for new ORR catalysts.More importantly,we reveal that this electronic descriptor can be extended to predict other CJ-structured nanoclusters.

关键词： single-atom catalysts crown-jewel oxygen reduction reaction(ORR) catalyst design nanocluster

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Systemic and single cell level responses to 1 nm size biomaterials demonstrate distinct biological effects revealed by multi-omics atlas

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Bioactive Materials 2022年第12期7卷 199-212页

作者： Tao Zhang Tingyun Lei Ruojin Yan Bo Zhou Chunmei Fan Yanyan Zhao Shasha Yao Haihua Pan Yangwu Chen Bingbing Wu Yuwei Yang Lijuan Hu Shen Gu Xiaoyi Chen Fangyuan Bao Yu Li Hanqi Xie Ruikang Tang Xiao Chen Zi Yin Dr.Li Dak Sum&Yip Yio Chin Center for Stem Cells and Regenerative Medicine and Department of Orthopedic Surgery of Sir Run Shaw HospitalZhejiang University School of MedicineHangzhou310058PR China Key Laboratory of Tissue Engineering and Regenerative Medicine of Zhejiang Province School of MedicineZhejiang UniversityHangzhou310058PR China China Orthopedic Regenerative Medicine Group CORMed Hangzhou310058PR China Department of Orthopaedic Surgery of Sir Run Run Shaw Hospital Zhejiang University School of MedicineHangzhou310058PR China Qiushi Academy for Advanced Studies Zhejiang UniversityHangzhou310058PR China Department of Pathology of the First Affiliated Hospital Anhui University of Chinese MedicineHefei230031PR China chool of Biomedical Sciences The Chinese University of Hong KongShatinN.THKSARChina

Although ultra-small nanoclusters(USNCs,<2 nm)have immense application capabilities in biomedicine,the investigation on body-wide organ responses towards USNCs is scant.Here,applying a novel strategy of single-cell mass cytometry combined with Nano Genome Atlas of multi-tissues,we systematically evaluate the interactions between the host and calcium phosphate(CaP)USNCs at the organism level.Combining single-cell mass cytometry,and magnetic luminex assay results,we identify dynamic immune responses to CaP USNCs at the single cell resolution.The innate immune is initially activated and followed by adaptive immune activation,as evidenced by dynamic immune cells proportions.Furthermore,using Nano Genome Atlas of multi-tissues,we uncover CaP USNCs induce stronger activation of the immune responses in the cartilage and subchondral bone among the five local tissues while promote metabolic activities in the liver and kidney.Moreover,based on the immunological response profiles,histological evaluation of major organs and local tissue,and a body-wide transcriptomics,we demonstrate that CaP USNCs are not more hazardous than the Food and Drug Administration-approved CaP nanoparticles after 14 days of injection.Our findings provide valuable information on the future clinical applications of USNCs and introduce an innovative strategy to decipher the whole body response to implants.

关键词： Nanoparticle nanocluster Single-cell mass cytometry RNA-Seq Multi-omics

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Kernels-Different Au_(25) nanoclusters Enhanced Catalytic Performance via Modification of Ligand and Electronic Effects

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Chinese Journal of Chemistry 2022年第21期40卷 2575-2581页

作者： Mei Qu Fang Xue Jiang-Yu Wei Miao-Miao Qiao Wei-Qi Ren Shi-Li Li Xian-Ming Zhang Key Laboratory of Magnetic Molecules and Magnetic Information of Ministry of Education School of Chemistry and Material ScienceShanxi Normal UniversityTaiyuanShanxi 030006China College of Chemistry Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan Universityof TechnologyTaiyuanShanxi 030024China

Ultrasmall atomically precise thiolate-protected gold nanoclusters with surface open sites are crucial for practical applications in catalysis.However,there is a lack of systematic studies that unify the kernels-isomerization,modification of peripheral ligands and electronic effects into one system,as well as their correlation to catalytic performances.In this work,three structurally related Au_(25)nanoclusters with reported star Au_(25) kernels,Au_(25)-i-FTP,Au_(25)-bi-FTP,and Au_(25)-bi-CHT have been synthesized through two different methods:one-pot direct reduction and two-step reduction by using AsPh3 as converter.Their structures and catalytic performance have been comparatively investigated.Au_(25)-i-FTP has a classic Au13 core capped by six dimeric RS-Au-SR-Au-SRs,while Au_(25)-bi-FTP and Au_(25)-bi-CHT feature typical rod-shaped biicosahedral geometric kernel.All of the three Au_(25) clusters were effective catalysts for oxidation of organosilanes,different from conclusions obtained in literature.Especially,the nanorod-type Au_(25)-bi-CHT clusters protected by flexible thiol ligands showed very good catalytic performance in this reaction,the conversion and selectivity were close to 100%within 5 min.The ligand rigidity and electron effects work together to modulate the catalytic properties.The findings inspire us to rethink kernel and ligand effects on catalytic property,and the principle demonstrated here will possibly be widely-used in high active atom-precise catalysts.

关键词： Gold nanocluster Atom-Precise Catalysis Silanols

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Co-based MoF derived metal catalysts: from nano-level to atom-level

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钨科技(英文) 2023年第2期5卷 201-216页

作者： Yuan-Xin Du Yan-Ting Zhou Man-Zhou Zhu College of Materials Science and Engineering and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials Department of Chemistry and Center for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of the Ministry of EducationAnhui UniversityHefei 230601China

Co-based metal-organic framework(MOF),a kind of porous crystal material composed of Co ions and organic linkers,is a common type of MOF.It not only has the intrinsic properties of MOF,such as structural diversity,functional adjustability,and high surface area,but more importantly,it contains Co metal species,which are considered by many reports to be active catalytic centers for many reactions.Meanwhile,metal catalysts always received wide and sustained attention.The combi-nation of the two types of catalysts can enhance the catalytic performance and achieve the"1+1>2"effect.In this review,we mainly overview the synthesis methods of Co-based MOF-derived metal catalysts from nano-to atom-level and their applications in the catalysis field in recent years and put forward our own views and prospects for this research direction.

关键词： Metal-organic framework Cobalt Catalysis Nanoparticle nanocluster Single-atom catalyst

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