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Aggregation-induced barrier to oxygen——a new AIE mechanism for metal clusters with phosphorescence

National Science Review 2022年第8期9卷 71-79页

作者： Yan Jin Qiu-Chen Peng Si Li Hui-Fang Su Peng Luo Ming Yang Xin Zhang Kai Li Shuang-Quan Zang Ben Zhong Tang Thomas C.W.Mak Henan Key Laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou University Shenzhen Institute of Aggregate Science and Technology School of Science and EngineeringChinese University of Hong Kong The Hong Kong Branch of the Chinese National Engineering Research Center for Tissue Restoration and Reconstruction Hong Kong University of Science and Technology Department of Chemistry Chinese University of Hong Kong

metal clusters are useful phosphors, but highly luminescent examples are quite rare. Usually, the phosphorescence of metal clusters is hindered by ambient O2molecules. Transforming this disadvantage into an advantage for meaningful applications of metal clusters presents a formidable challenge. In this work, we used ligand engineering to judiciously prepare colour-tuneable and brightly emitting Cu(I)clusters that are ultrasensitive to O2upon dispersion in a fluid solution or in a solid matrix. When the O2scavenger dimethyl sulfoxide(DMSO) was used as the solvent, joint photo-and oxygen-controlled multicolour switches were achieved for the first time for metal cluster-based photopatterning and photo-anticounterfeiting. More importantly, an aggregation-induced barrier to oxygen, a new aggregation-induced emission mechanism for metal clusters, was proposed, providing a new pathway to realizing the intense emission of metal clusters in the aggregated state. These results are expected to promote the application of metal clusters and enrich the luminescence theory of metal cluster aggregates.

关键词： metal clusters aggregation-induced emission phosphorescence photoresponse O_2 detection

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Preparation and Reaction of Naked metal clusters for Catalysis and Genetic Materials

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Chinese Journal of Structural Chemistry 2020年第6期39卷 989-998页

作者：崔超男张含宇骆智训潘锋 Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Stnictural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China School of Advanced Materials Peking University Shenzhen Graduate SchoolShenzhen 518055China

metal clusters that contain a small number of atoms usually present unique properties with dramatic dependence on their sizes,geometric structures,and *** studies of naked metal clusters are devoted to develop new catalysts and functional materials of atomic precision,and enable to improve the fundamental theory of structure chemistry and to understand the basic reactions and properties bridging the gap between atoms and bulk *** particular,some interesting superatom clusters have received reasonable research interest indicative of materials gene of *** in this review,we simply summarize the preparation,stability,and reactivity of naked metal clusters with a few examples *** it serves as a modest spur to stimulate more interest of related investigations in this field.

关键词： metal clusters structure chemistry superatom cluster reactivity

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Growth Mechanism of metal clusters and Molecules on a Graphene/Ru(0001)Template

Growth Mechanism of Metal Clusters and Molecules on a Graphe...

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中国真空学会2014学术年会

作者： Shixuan Du Institute of Physics Chinese Academy of Sciences

Due to the soft nature of epitaxial graphene and the lattice mismatch between graphene and metal substrates periodic moire patterns can be formed.A graphene/metal template,moire template,can be used to grow dispersed metal nano-clusters with controllable size and shape,metal clusters with large size and metal layers,or ordered functional molecular ***,how intrinsic properties of metal atoms(or functional molecules)and the moire template influence the selective adsorption and the growth mode of metal clusters and the molecules is still open to debate.A general rule,predicting the morphology of metal nano-clusters and molecules on a G/metal surface,important to guide experimenters,is still *** first-principles calculations combined with scanning tunneling microscopy experiments,we investigated the adsorption configurations,electronic structures and the corresponding growth mechanism of several transition metal(TM)atoms and two kinds of molecules on a graphene/Ru(0001)moire template(G/Ru(0001))at low *** transition metal atoms,we find that both the unoccupied d orbital of the TM atoms and the strong sp hybridization of carbon atoms in the fcc region of G/Ru(0001)determine the growth mode because of the strong *** molecules,due to the weak interaction between molecules and the substrate,the selective adsorption behavior is determined by the lateral dipole *** simulations agree well with the experimental ***,it also provides guidance for the selection of suitable metal atoms or molecules to form ordered dispersed structures on similar templates.

关键词： Graphene metal clusters functional molecules selective adsorption

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Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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Carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State Key Laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

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Structural Isomerization in Cu(I)clusters:Tracing the Cu Thermal Migration Paths and Unveiling the Structure-Dependent Photoluminescence

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CCS Chemistry 2023年第2期5卷 350-360页

作者： Xi Fan Furong Yuan Jiaqi Wang Zhibin Cheng Shengchang Xiang Huayan Yang Zhangjing Zhang Fujian Provincial Key Laboratory of Polymer Materials College of Chemistry and Materials ScienceFujian Normal UniversityFuzhouFujian 350007 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 Health Science Center School of Biomedical Engineering Shenzhen UniversityShenzhen 518000

Revealing structural isomerization in metal clusters would bridge a huge structural gap between small molecular isomerization and solid–solid phase ***,genuine structural isomerism in metal clusters is still *** this work,we report the first example of structural isomerismin Cu *** utilizing the coordination flexibility of alkyne to enable the migration of partial Cu atoms in Cu metal cores,two Cu_(15)cluster complexes(Cu_(15)-a and Cu_(15)-c)possessing identical composition but different metal core structures have been successfully ***,although the structure of Cu_(15)-a can be retained in CH_(2)C_(l2)solution below 27°C,it will gradually change to give an intermediate state,Cu_(15)-b,as the temperature rises(at about 31°C)before it eventually transforms into Cu_(15)-c(at 40∼65°C).Significantly,atomically precise Cu_(15)-b clearly provides footprints for tracing the thermal migration process of Cu atoms during the thermal transformation from Cu_(15)-a to Cu_(15)-*** addition,Cu_(15)-a and Cu_(15)-c exhibit diverse crystallization-induced emission enhancement *** Cu_(15)-c displays redshifted photoluminescence(820 nm)compared with Cu_(15)-a(726 nm)due to the shorter mean Cu···Cu distance in Cu_(15)-***,crystalline Cu_(15)-a exhibits much more intense photoluminescence at room temperature than that in Cu_(15)-c,which might be attributed to the stronger intermolecular C–H⋯πinteractions in Cu_(15)-*** results indicate that cluster isomerism provides valuable opportunities for insight into the structure–property relationships and understanding the complex evolution of phase transformation in nanometallic solids.

关键词： cluster compounds metal clusters structural isomerism isomeric transformation structure–property relationships

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Wet-milling synthesis of immobilized Pt/Ir nanoclusters as promising heterogeneous catalysts

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Nano Research 2022年第4期15卷 3065-3072页

作者： Peng Du Kai Huang Xiaoyuan Fan Jingteng Ma Naveed Hussain Ruyue Wang Bohan Deng Binghui Ge Haolin Tang Ru Zhang Ming Lei Hui Wu State Key Laboratory of Information Photonics and Optical Communications&School of Science Beijing University of Posts and TelecommunicationsBeijing 100876China State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Institutes of Physical Science and Information Technology Anhui UniversityHefei 230601China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Being a typical state of the art heterogeneous catalyst,supported noble metal catalyst often demonstrates enhanced catalytic ***,a facile synthetic method for realizing large-scale and low-cost supported noble metal catalyst is strictly *** this end,by making use of the strong metal-support interaction(SMSI)and mechanochemical reaction,we introduce an efficient synthetic route to obtain ultrafine Pt and Ir nanoclusters immobilized on diverse substrates by wet chemical *** further demonstrate the scaling-up effect of our approach by large-scale ball-milling production of Pt nanoclusters immobilized on TiO_(2)*** synthesized Pt/Ir@Co_(3)O_(4)catalysts exhibit superior oxygen evolution reaction(OER)performance with only 230 and 290 mV overpotential to achieve current density of 10 and 100 mA·cm^(-2),beating the catalytic performance of Co_(3)O_(4)supported Pt or Ir clusters and commercial Ir/*** is envisioned that the present work strategically directs facile ways for fabricating supported noble metal heterogeneous catalysts.

关键词： heterogeneous catalysts metal clusters wet milling large-scale production strong metal–support interaction

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Halide Anchors for Single-Cluster Electronics

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CCS Chemistry 2023年第7期5卷 1574-1582页

作者： Caiyun Wei Jingyao Ye Yuming Su Jueting Zheng Siqiang Xiao Jiawei Chen Saisai Yuan Chengyang Zhang Jie Bai Han Xu Jia Shi Jiale Huang Wenjing Hong State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005

Due to their unique electronic structure,well-defined metal clusters at the atomic level are promising materials for single-cluster ***,coupling between the electrode and the cluster remains challenging mainly due to the coverage of bulky ligands on the noble *** the scanning tunneling microscopy break junction(STM-BJ)technique,we have developed a“direct contact”approach to fabrication and investigation of the charge transport through single-cluster junctions of AgCu bimetallic metal clusterswith different halide *** that the electrodes could make contact directly with the surface halides of the single-cluster junctions and experience different contact resistance from different halogen *** and calculations reveal that the halide anchors provided efficient coupling between the cluster and the electrode,and the enhanced coupling with various halide anchors promoted electron transport and improved transmission *** work offers a“direct contact”strategy for interface design between clusters of noble metals and electrodes,an essential step in progress toward single-cluster electronics.

关键词： single-cluster junctions metal clusters halide anchoring site coupling strength

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Unique Magnetic Moment and Electronic Properties for Fe（MgO）n（n=1-8） clusters： First-Principles Calculations

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Chinese Physics Letters 2009年第8期26卷 98-101页

作者：葛桂贤井群杨增强罗有华 Key Laboratory of Ecophysics and Department of Physics Normal College Shihezi University Xinjiang 832003 School of Science East China University of Science and Technology Shanghai 200237- Institute for Theoretical Physics Henan University Kaifeng 475001

The geometries and electronic properties of Fe（MgO）n are systematically investigated by the density functional theory. The results show that the doped Fe atom is prone to bond with the O atom, and Fe almost does not disturb the frame of （MgO）n. The second-order energy difference, the fragmentation energies and the electron amnities show that Fe（MgO）4 and Fe（MgO）6 possess relatively higher stabilities. The HOMO-LUMO gaps of Fe（MgO）n decrease obviously as compared with （MgO）n. Almost equal unpaired electrons of the 3d state of the Fe atom in Fe（MgO）n result in a nearly equal magnetic moment of Fe（MgO）n.

关键词： MAGNETIC dipoles ELECTRONIC structure IRON compounds metal clusters DENSITY functionals CHEMICAL affinity NUCLEAR fragmentation

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A Parallel Study on （BN）n and （HAlNH）n （n=11-22） clusters： Geometry and Stability

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Chinese Physics Letters 2009年第3期26卷 87-90页

作者：蹇国强陈新胡征 Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical Engineering Nanfing University Nanjing 210093

A parallel study on （BN）n and （HAlNH）n （n = 11-22） clusters is presented herein with ab initio HF/6-31G^＊ method. Two types of structures, i.e. cage-like and needle-shaped, are constructed. The calculated results indicate that the classical cage-like geometry is energetically more favourable for （BN）n while the needle-shaped （HAlNH）n structures are more stable than their cage-like counterparts. It is suggested that the nanostructures with higher structural similarity to the corresponding bulk phases possess greater stability. This idea leads to the viable way to intercept segment from bulk materials to construct models for theoretical study of complex nanostructures.

关键词： metal clusters ORGANOmetalLIC compounds CHEMICAL structure NANOSTRUCTURES CHEMICAL models STRUCTURAL analysis (Science) BULK solids CHEMISTRY -- Mathematics

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Copper-hydride nanoclusters with enhanced stability by N- heterocyclic carbenes

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Nano Research 2021年第9期14卷 3303-3308页

作者： Hui Shen Lingzheng Wang Omar Lopez-Estrada Chengyi Hu Qingyuan Wu Dongxu Cao Sami Malola Boon KTeo Hannu Hakkinen Nanfeng Zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsNational&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Departments of Physics and Chemistry Nanoscience CenterUniversity ofjyvdskyldFI-40014 JyvdskyldFinland

Copper-hydrides have been intensively studied for a long time due to their utilization in a variety of technologically important chemical ***,poor stability of the species severely hinders its isolation,storage and operation,which is worse for nano-sized *** report here an unprecedented strategy to access to ultrastable copper-hydride nanoclusters(NCs),namely,using bidentate N-heterocyclic carbenes as stabilizing ligands in addition to *** this work,a simple synthetic protocol was developed to synthesize the first large copper-hydride nanoclusters(NCs)stabilized by N-heterocyclic carbenes(NHCs).The NC,with the formula of Cu3i(RS)25(NHC)3H6(NHC=1,4-bis(1-benzyl-1 H-benzimidazol-1-ium-3-yl)butane,RS=4-fluorothiophenol),was fully characterized by high resolution Fourier transform ion cyclotron resonance mass spectrum,nuclear magnetic resonance,ultra-violet visible spectroscopy,density functional theory(DFT)calculations and single-crystal X-ray ***,the title cluster exhibits unprecedented Cu4 tetrahedron-based vertex-sharing(TBVS)superstructure(fusion of six Cu4 tetrahedra).Moreover,the ultrahigh thermal stability renders the cluster a model system to highlight the power of NHCs(even other carbenes)in controlling geometrical,electronic and surface structure of polyhydrido copper clusters.

关键词： metal clusters copper-hydride N-hetercxylic carbene stability superatom

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