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学者姓名：李新雄
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Abstract ：
Lanthanide ion contained metal-organic frameworks (MOFs) have garnered significant attention in the fields of solid-state lighting and chemical sensing due to their porous structure and distinctive optical properties. However, they also present challenges because of the limited photoluminescence (PL) intensity resulting from the parity-forbidden f-f transitions of lanthanide ions. Herein, the study reports a new heterometallic MOFs Ln3Li2L4 (Li-Ln-MOF, Ln = Y, Eu, Tb and Dy, L = deprotonated 1,3,5-tris(4-carboxyphenyl)benzene) with a Brunauer-Emmett-Teller (BET) surface area of 774.1 m2/g. The porous crystal structure of Li-Ln-MOF is characterized by three kinds of channels interpenetrating with each other. By employing ligand alternation and lanthanide ion alloying strategies, Li-Y1-xEux-MOF1 crystal isostructural with Li-Ln-MOF is synthesized by using 2,4,6-tris(4-carboxyphenyl)-1,3,5-triazine (H3TATB) as ligand. The Li-Y0.7Eu0.3-MOF1 crystal excels in the comprehensive performance with a BET surface area of 858.8 m2 g-1 and a near-unity PL quantum yield. The time density functional theory and natural transition orbitals calculations unravel that the outstanding optical properties Li-Y0.7Eu0.3-MOF1 originates from the charge transfer between TATB3- and Eu3+. Benefiting from the excellent comprehensive performance of Li-Y1-xEux-MOF1, the study reveals their potentials as single-composition white-light emission and fluorescent sensing probe for the detection of nitrobenzene. A strategy via ligand alteration is developed to achieve a near-unity photoluminescence quantum yield in lanthanide metal-organic frameworks (Ln-MOFs) with a porosity of up to 53.6%. Mechanistic investigation through theoretical calculation and time-resolved spectra unravel that Ln-MOF displayed outstanding optical properties ascribed to the charge transfer from the triple excited state of ligand to the Ln3+. image
Keyword ：
fluorescent sensing fluorescent sensing lanthanide-organic frameworks lanthanide-organic frameworks ligand alteration ligand alteration photoluminescence photoluminescence white-light emission white-light emission
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| GB/T 7714 | Zhang, Wei , Wang, En-Ting , Li, Xinhao et al. Lithium-Lanthanide Heterometallic Organic Frameworks with Near-Unity Photoluminescence Quantum Yields for Single-Composition White-Light Emission and Fluorescent Sensing on Nitrobenzene [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (21) . |
| MLA | Zhang, Wei et al. "Lithium-Lanthanide Heterometallic Organic Frameworks with Near-Unity Photoluminescence Quantum Yields for Single-Composition White-Light Emission and Fluorescent Sensing on Nitrobenzene" . | ADVANCED OPTICAL MATERIALS 12 . 21 (2024) . |
| APA | Zhang, Wei , Wang, En-Ting , Li, Xinhao , Huang, Weixin , Sun, Yakun , Liu, Zheyuan et al. Lithium-Lanthanide Heterometallic Organic Frameworks with Near-Unity Photoluminescence Quantum Yields for Single-Composition White-Light Emission and Fluorescent Sensing on Nitrobenzene . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (21) . |
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Herein, we report the synthesis, crystal structure, and optical properties of a metal-free three-dimensional (3D) inorganic covalent framework ((H(2)en)-[Si-(B4O9)], named CityU-11, where H(2)en is the abbreviation for ethanediamine). With the assistance of a tiny amount of F- ions and the selection of SiO2 as Si sources, single crystals of CityU-11 can be successfully prepared under solvothermal conditions. The precise structure information on CityU-11 has been disclosed through both single-crystal X-ray diffraction (SCXRD) and low-dose high-resolution transmission electron microscopy (LD-HRTEM). The SCXRD results showed that CityU-11 crystallized in the noncentrosymmetric space group of Pnn2, while LD-HRTEM suggested that CityU-11 possessed almost the same interplanar distances of 0.6 nm for both (200) and (020) crystal planes, which finely matched with the double peaks of 2 theta = 15 degrees in the pattern of its powder X-ray diffraction (PXRD). CityU-11 also displayed an interesting optical property with a moderate birefringence of 0.0258@550 nm.
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| GB/T 7714 | Dong, Qiang , Zhang, Lei , Chen, Cailing et al. Borosilicate-Based Framework: Synthesis, Single-Crystal Structure Study, and Physical Properties [J]. | INORGANIC CHEMISTRY , 2024 , 63 (5) : 2663-2669 . |
| MLA | Dong, Qiang et al. "Borosilicate-Based Framework: Synthesis, Single-Crystal Structure Study, and Physical Properties" . | INORGANIC CHEMISTRY 63 . 5 (2024) : 2663-2669 . |
| APA | Dong, Qiang , Zhang, Lei , Chen, Cailing , Xue, Miaomiao , Zhu, Zengkui , Wang, Xiang et al. Borosilicate-Based Framework: Synthesis, Single-Crystal Structure Study, and Physical Properties . | INORGANIC CHEMISTRY , 2024 , 63 (5) , 2663-2669 . |
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Two types of isostructural iron-cobalt/nickel-antimony-oxo tartrate cluster-based compounds, namely (H3O)(Me2NH2)[M(H2O)6]2[FeII2SbIII12(mu 4-O)3(mu 3-O)8(tta)6]center dot 6H2O (M = Co (1); Ni (3)), H5/3[Co2.5FeII4/3FeIII3(H2O)13SbV1/3FeIII2/3(mu 4-O)2(mu 3-O)4SbIII6(mu 3-O)2(tta)6]center dot 2H2O (2) and H2[Ni2.25FeII1.5FeIII3(H2O)14SbV0.25FeIII0.75(mu 4-O)2(mu 3-O)4SbIII6(mu 3-O)2(tta)6]center dot 2H2O (4) (H4tta = tartaric acid) were synthesized via simple solvothermal reactions. All the clusters in the structures adopt sandwich configurations, that is, bilayer sandwich configuration in 1 and 3 and monolayer sandwich configuration in 2 and 4. Interestingly, the monolayer sandwiched compounds 2 and 4 represent rare examples of cluster-based compounds containing mixed-valence Sb(III, V), whose center of the intermediate layer is the co-occupied [FexSbV1-x]. This is different from that of previously reported sandwich-type antimony-oxo clusters in which the center position is either occupied by a transition metal ion or a Sb(V) alone. Thus, the discovery of title compounds 2 and 4 makes the evolution of center metal ion more complete, that is, from M, MxSbV1-x to SbV. All the title compounds were fully characterized, and the photocatalysis, proton conduction and magnetism of compounds 2 and 4 were studied.
Keyword ：
antimony-oxo cluster antimony-oxo cluster magnetism magnetism mixed-valence mixed-valence photodegradation photodegradation proton conduction proton conduction transition metal transition metal
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| GB/T 7714 | Wen, Weiyang , Wang, Yanqi , Pan, Tianyu et al. Synthesis and Properties of Cobalt/Nickel-Iron-Antimony(III, V)-Oxo Tartrate Cluster-Based Compounds [J]. | MOLECULES , 2024 , 29 (3) . |
| MLA | Wen, Weiyang et al. "Synthesis and Properties of Cobalt/Nickel-Iron-Antimony(III, V)-Oxo Tartrate Cluster-Based Compounds" . | MOLECULES 29 . 3 (2024) . |
| APA | Wen, Weiyang , Wang, Yanqi , Pan, Tianyu , Hu, Qianqian , Xiao, Huiping , Wang, Nannan et al. Synthesis and Properties of Cobalt/Nickel-Iron-Antimony(III, V)-Oxo Tartrate Cluster-Based Compounds . | MOLECULES , 2024 , 29 (3) . |
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In this work, a novel organodiphosphate-containing inorganic-organic hybrid polyoxoniobate (PONb) ring {(PO3CH2CH2PO3H)(4)Nb8O16}(4-) (Nb8P8) has been achieved by a one-pot hydrothermal method. The ring is constructed from a tetragonal {Nb8O36} motif and four {PO3CH2CH2PO3H} ligands. Interestingly, Nb8P8 can be joined together via K-H2O clusters {K-2(H2O)(4)(OH)(2)} to form one-dimensional chains {[K-2(H2O)(4)(OH)(2)]Nb8P8}(n) and further linked by {Cu(en)(2)}(2+) (en = ethylenediamine) complexes, resulting in a three-dimensional supramolecular framework {[Cu(en)(2)](2)[K-2(H2O)(4)(OH)(2)]Nb8P8}3enH2O (1). 1 exhibits good chemical and thermal stability and has a high water vapor adsorption capacity of <= 224 cm(3) g(-1) (22.71 molmol(-1)) at 298 K, outperforming most of the known polyoxometalate-based materials. Impedance measurements prove that 1 can transfer protons with moderate conductivity. This study not only contributes to the structural diversity of organodiphosphate-containing PONbs and PONb rings but also provides a reference for the development of PONb-based materials with unique performance.
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| GB/T 7714 | Cong, Yu-Chen , Xiao, Hui-Ping , Cai, Ping-Wei et al. An Organodiphosphate-Containing Polyoxoniobate Ring and Its Assembly into a Three-Dimensional Framework through Hydrogen Bonding [J]. | INORGANIC CHEMISTRY , 2024 , 63 (20) : 9204-9211 . |
| MLA | Cong, Yu-Chen et al. "An Organodiphosphate-Containing Polyoxoniobate Ring and Its Assembly into a Three-Dimensional Framework through Hydrogen Bonding" . | INORGANIC CHEMISTRY 63 . 20 (2024) : 9204-9211 . |
| APA | Cong, Yu-Chen , Xiao, Hui-Ping , Cai, Ping-Wei , Sun, Cai , Sun, Yan-Qiong , Qi, Ming-Qiang et al. An Organodiphosphate-Containing Polyoxoniobate Ring and Its Assembly into a Three-Dimensional Framework through Hydrogen Bonding . | INORGANIC CHEMISTRY , 2024 , 63 (20) , 9204-9211 . |
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By variation of the amount of GeO2, two organic-inorganic hybrid germanoniobate frameworks with 6-connected pcu and 10-connected bct topologies were constructed from peanut-shaped {alpha-Ge12Nb38} and {beta-Ge12Nb38} clusters, respectively. The {alpha-Ge12Nb38} and {beta-Ge12Nb38} clusters contain the most Ge centers of germanoniobates reported so far. The compounds exhibit proton conduction properties with a conductivity of 3.04 x 10(-4) Scm(-3) for 1 and 1.62 x 10(-4) Scm(-3) for 2 at 85 degrees C and 98% RH. The water vapor adsorption capacities for 1 and 2 are 5.86 and 4.40 mmolg(-1), respectively.
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| GB/T 7714 | Wang, Yong-Jiang , Yu, Lan , Li, Xin-Xiong et al. Two Unprecedented Germanoniobate Frameworks Based on High-Nuclearity Peanut-Shaped {Ge12Nb38} Clusters [J]. | INORGANIC CHEMISTRY , 2024 , 63 (2) : 1388-1394 . |
| MLA | Wang, Yong-Jiang et al. "Two Unprecedented Germanoniobate Frameworks Based on High-Nuclearity Peanut-Shaped {Ge12Nb38} Clusters" . | INORGANIC CHEMISTRY 63 . 2 (2024) : 1388-1394 . |
| APA | Wang, Yong-Jiang , Yu, Lan , Li, Xin-Xiong , Sun, Yan-Qiong , Zheng, Shou-Tian . Two Unprecedented Germanoniobate Frameworks Based on High-Nuclearity Peanut-Shaped {Ge12Nb38} Clusters . | INORGANIC CHEMISTRY , 2024 , 63 (2) , 1388-1394 . |
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An inorganic hexalanthanide-oxo-cluster-encapsulated antimotungstate, K2Na3H43[Nd6(OH)6(H2O)6(B-alpha-SbW9O33)4]2 center dot 67H2O (1), has been successfully synthesized by a facile one-step hydrothermal reaction method. The tetrahedron-shaped two-shell {Nd6(OH)6(H2O)6(B-alpha-SbW9O33)4}(1a) polyanion is composed of a novel pure lanthanide-oxo {Nd6(mu 3-OH)6(H2O)6} octahedron and {(B-alpha-SbW9O33)4} tetrahedron. After being effectively loaded onto a glassy carbon electrode (GCE) by electrostatic adsorption using polydiallyldimethyl ammonium chloride (PDDA)-functionalized multi-walled carbon nanotubes (MWCNTs), compound 1 exhibits electrochemical activity for the reduction of bromate ions with good selectivity, a high sensitivity of 186 mu A mM-1 and a detection limit that has reached 1.9 mu M. To the best of our knowledge, this is the first example of an amperometric bromate sensor based on Ln-containing antimotungstates, which will provide new materials for electrochemical sensors. An inorganic antimotungstate 1 is constructed from tetrahedron-shaped two-shell {Nd6(OH)6(H2O)6(B-alpha-SbW9O33)4} polyanions. Compound 1 exhibits electrochemical activity for the reduction of BrO3- with good selectivity, high sensitivity and low detection limit.
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| GB/T 7714 | Yu, Lan , Ye, Jing , Li, Da-Huan et al. A tetrahedron-shaped polyoxoantimotungstate encapsulating a hexanuclear octahedral lanthanide-oxo cluster for an amperometric bromate sensor [J]. | DALTON TRANSACTIONS , 2024 , 53 (11) : 5258-5265 . |
| MLA | Yu, Lan et al. "A tetrahedron-shaped polyoxoantimotungstate encapsulating a hexanuclear octahedral lanthanide-oxo cluster for an amperometric bromate sensor" . | DALTON TRANSACTIONS 53 . 11 (2024) : 5258-5265 . |
| APA | Yu, Lan , Ye, Jing , Li, Da-Huan , Sun, Yan-Qiong , Li, Xin-Xiong , Zheng, Shou-Tian . A tetrahedron-shaped polyoxoantimotungstate encapsulating a hexanuclear octahedral lanthanide-oxo cluster for an amperometric bromate sensor . | DALTON TRANSACTIONS , 2024 , 53 (11) , 5258-5265 . |
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Polyoxometalate (POM)-based materials are ideal candidates for implementing molecular memories, and rational POM molecule design is key to higher resistive switching (RS) performance. In this work, in order to obtain a deep structure-property correlation of POM-based memristors, three Anderson-based hybrids, i.e. two-component hybrids (MV)3(MnMo6O18L2)2·4DMF (1) and (MV)2[Cu(DMF)2](MnMo6O18L1)2·6DMF (2), and the three-component one (MV)2(Cu2I3)(MnMo6O18L2)·4CH3CN (3) (L = 2-(hydroxymethyl)-2-(pyridine-4-yl)-1,3-propanediol) have been structurally determined. These hybrids together with the precursors (methyl viologen (MV2+), CuI, and (MnMo6O18L2)) were further fabricated as memristors with the structure of ITO/active layer/Ag. Interestingly, three precursors are RS silent or have bad RS performance, but the incorporation of MV2+ in 1 and 2 can trigger the RS performances, and the further decoration of iodocuprate in 3 can render enhanced RS behavior (ON/OFF ratio: 2.32 × 102) with high thermal-tolerance temperature (240 °C) and extremely long-term stability. The RS mechanism could be assigned to the valence change (VC) induced by oxygen vacancy migrations. The presence of air-stable (MnMo6O18L2)3−-MV2+ donor-acceptor couples can stabilize the oxygen vacancies, which not only trigger the RS behaviors in ITO/1/Ag and ITO/2/Ag, but also result in extremely long-term stability in ITO/3/Ag. Besides, the oxygen vacancies can also be stabilized by Cu2I3 with intense cuprophilic interactions, which corresponds to enhanced RS properties in ITO/3/Ag. This mechanism could be validated by the following structural characters in 3: the stronger POM-MV2+ interactions, the better planarity of MV2+, the very short Cu⋯Cu distances and the ABAB-type packing fashion. The structure-property correlation in this work can provide a new strategy for the development of highly efficient and reliable memristors. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Chen, H.-B. , He, M.-Y. , Li, T. et al. Exploring the role of viologen and iodocuprate in the enhanced resistive switching performance of Anderson polyoxometalate-based three-component hybrids [J]. | Journal of Materials Chemistry C , 2024 , 12 (34) : 13555-13561 . |
| MLA | Chen, H.-B. et al. "Exploring the role of viologen and iodocuprate in the enhanced resistive switching performance of Anderson polyoxometalate-based three-component hybrids" . | Journal of Materials Chemistry C 12 . 34 (2024) : 13555-13561 . |
| APA | Chen, H.-B. , He, M.-Y. , Li, T. , Deng, C.-C. , Xiao, H.-P. , Qi, M.-Q. et al. Exploring the role of viologen and iodocuprate in the enhanced resistive switching performance of Anderson polyoxometalate-based three-component hybrids . | Journal of Materials Chemistry C , 2024 , 12 (34) , 13555-13561 . |
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Nature seems to favor the formation of closed anion-templated silver clusters. How precisely to create non-closed sliver clusters remains an interesting challenge. In this work, we propose that the use of transition-metal-coordination-cluster substituted polyoxometalates (TMCC-substituted POMs) as templates is an effective synthetic strategy for creating the non-closed silver clusters, as demonstrated by the obtainment of four types of rare non-closed silver cluster species of Ag38-TM (TM = Co, Ni or Zn), Ag37-Zn, {Ag37-Zn}∞ and Ag36-TM (TM = Co, Ni). The idea of the strategy is to employ the TMCC-substituted POMs containing cluster modules with different bond interactions with Ag+ ions as templates to guide the formation of the non-closed silver clusters. For example, TMCC-substituted POM clusters are used as templates in this work, which contain POM modules that can coordinate with the Ag+ ions and TMCC moieties that are difficult to coordinate with the Ag+ ions, leading to the Ag+ ions being unable to form closed clusters around TMCC-substituted POM templates. The work demonstrates a promising approach to developing intriguing and unexplored non-closed silver clusters. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Ge, R. , Cai, P.-W. , Sun, C. et al. Development of non-closed silver clusters by transition-metal-coordination-cluster substituted polyoxometalate templates [J]. | Chemical Science , 2024 , 15 (31) : 12543-12549 . |
| MLA | Ge, R. et al. "Development of non-closed silver clusters by transition-metal-coordination-cluster substituted polyoxometalate templates" . | Chemical Science 15 . 31 (2024) : 12543-12549 . |
| APA | Ge, R. , Cai, P.-W. , Sun, C. , Sun, Y.-Q. , Li, X.-X. , Zheng, S.-T. . Development of non-closed silver clusters by transition-metal-coordination-cluster substituted polyoxometalate templates . | Chemical Science , 2024 , 15 (31) , 12543-12549 . |
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An unusual crystalline porous framework constructed from four types of cages, including all-inorganic Keggin-type polyoxometalate (POM) cages [H3W12O40](5-), organic hexamethylenetetramine (Hmt) cages, nanosized silver-Hmt coordination cages, and giant POM-silver-Hmt cages, was hydrothermally synthesized and structurally characterized. The framework features a highly symmetrical structure with one-dimensional nanoscale channels and holds good thermal/solvent stability, which endow it with proton conduction properties and heterogeneous catalytic activity for pyrazole. This paper not only contributes to broadening the structural diversity of cage-based crystalline porous framework materials but also sheds new light on the design of new functional framework materials.
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| GB/T 7714 | Ma, Xiao-Qi , Liu, Yu-Feng , Yang, Guo-Ping et al. An Unusual Crystalline Porous Framework Constructed from Multitypes of Cages with Proton Conduction Property and Heterogeneous Catalytic Activity for Pyrazole Synthesis [J]. | INORGANIC CHEMISTRY , 2024 , 63 (26) : 12240-12247 . |
| MLA | Ma, Xiao-Qi et al. "An Unusual Crystalline Porous Framework Constructed from Multitypes of Cages with Proton Conduction Property and Heterogeneous Catalytic Activity for Pyrazole Synthesis" . | INORGANIC CHEMISTRY 63 . 26 (2024) : 12240-12247 . |
| APA | Ma, Xiao-Qi , Liu, Yu-Feng , Yang, Guo-Ping , Kong, Xiang-Jian , Li, Xin-Xiong , Zheng, Shou-Tian . An Unusual Crystalline Porous Framework Constructed from Multitypes of Cages with Proton Conduction Property and Heterogeneous Catalytic Activity for Pyrazole Synthesis . | INORGANIC CHEMISTRY , 2024 , 63 (26) , 12240-12247 . |
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Atomically precise low-nuclearity (n<10) silver nanoclusters (AgNCs) have garnered significant interest due to their size-dependent optical properties and diverse applications. However, their synthesis has remained challenging, primarily due to their inherent instability. The present study introduces a new feasible approach for clustering silver ions utilizing highly negative and redox-inert polyoxoniobates (PONbs) as all-inorganic ligands. This strategy not only enables the creation of novel Ag-PONb composite nanoclusters but also facilitates the synthesis of stable low-nuclearity AgNCs. Using this method, we have successfully synthesized a small octanuclear rhombic [Ag-8](6+) AgNC stabilized by six highly negative [LiNb27O75](14-) polyoxoanions. This marks the first PONb-protected superatomic AgNC, designated as {Ag-8@(LiNb27O75)(6)} (Ag-8@Nb-162), with an aesthetically spherical core-shell structure. The crystalline Ag-8@Nb-162 is stable under ambient conditions, What's more, it is water-soluble and able to maintain its molecular cluster structure intact in water. Further, the stable small [Ag-8](6+) AgNC has interesting temperature- and pH-dependent reversible fluorescence response, based on which a multiple optical encryption mode for anti-counterfeit technology was demonstrated. This work offers a promising avenue for the synthesis of fascinating and stable PONb-protected AgNCs and sheds light on the development of new-type optical functional materials.
Keyword ：
fluorescence fluorescence macromolecules macromolecules nanoclusters nanoclusters polyoxoniobate polyoxoniobate silver silver
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| GB/T 7714 | Hong, Li-Hao , Yue, Sheng-Nan , Huang, Xing et al. Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
| MLA | Hong, Li-Hao et al. "Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 29 (2024) . |
| APA | Hong, Li-Hao , Yue, Sheng-Nan , Huang, Xing , Sun, Cai , Cai, Ping-Wei , Sun, Yan-Qiong et al. Development of Stable Water-Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate-Protected Strategy: Giant Core-Shell-Type Ag8@Nb162 Fluorescent Nanocluster . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
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