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学者姓名：李新雄
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Abstract ：
A series of novel cage-like transition-metal (TM) incorporated heteropolyoxoniobates {TM4Nb64O200} (1-TM, TM = Ni, Cu, Mn, Cd) were hydrothermally synthesized and isolated as salts of mixed K+ and [CN3H6]+. As a result of transition metal ions incorporation, the charge distribution, redox potential, and active sites of the formed polyoxoniobates (PONbs) are variants, leading to differences in their electrocatalytic hydrogen evolution reaction (HER). Among these compounds, 1-Ni showed the best HER activity with an overpotential of 560 mV at 10 mA cm-2 and a minimum Tafel slope of 405.8 mV dec-1.
Keyword ：
Cage-like Cage-like Hydrogen evolution reaction Hydrogen evolution reaction Polyoxometalate Polyoxometalate Transition metal substitution Transition metal substitution
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| GB/T 7714 | Wu, Lan , Hu, Fen , Sun, Rong-Zhi et al. Development of cage-like transition-metal incorporated polyoxoniobates for hydrogen evolution reaction electrocatalysts [J]. | JOURNAL OF SOLID STATE CHEMISTRY , 2025 , 345 . |
| MLA | Wu, Lan et al. "Development of cage-like transition-metal incorporated polyoxoniobates for hydrogen evolution reaction electrocatalysts" . | JOURNAL OF SOLID STATE CHEMISTRY 345 (2025) . |
| APA | Wu, Lan , Hu, Fen , Sun, Rong-Zhi , Xia, Wen-Jun , Zeng, Qing-Xin , Cai, Ping-Wei et al. Development of cage-like transition-metal incorporated polyoxoniobates for hydrogen evolution reaction electrocatalysts . | JOURNAL OF SOLID STATE CHEMISTRY , 2025 , 345 . |
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A Tm(III)-rich silicotungstate Na{Tm3(H2O)17[Tm2(H2O)7(Si2W18O66)]}35H2O (Tm 5 Si 2 W 18 ) based on the open Wells-Dawson-type [Si2W18O66]16- building unit was synthesized by the reaction of Na10[alpha-SiW9O34]18H2O, itaconic acid, and TmCl3 in a HAc/NaAc buffer solution. Five kinds of Tm(III) ions were found in this compound and further linked the {Tm2Si2W18} subunit to form an interesting wavy 1D chain structure, which achieved the introduction of more lanthanide (Ln) ions into the [Si2W18O66]16- unit for the first time. Tm 5 Si 2 W 18 contains multiple exposed Tm-metal active sites, making it an efficient catalyst for the acetalization of 2-aminobenzamides/2-aminobenzenesulphonamides with aldehydes. A series of 2,3-dihydroquinazolinones and 3,4-dihydro-2H-1,2,4-benzothiadiazine-1,1-dioxides could be obtained in excellent yields under green and mild conditions.
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| GB/T 7714 | Yang, Guoping , Cao, Jiawei , Xiao, Yu et al. A Wavy Multiple Tm(III)-Containing Open Wells-Dawson Silicotungstate: Synthesis, Structure, and Catalytic Application [J]. | INORGANIC CHEMISTRY , 2025 , 64 (2) : 1041-1047 . |
| MLA | Yang, Guoping et al. "A Wavy Multiple Tm(III)-Containing Open Wells-Dawson Silicotungstate: Synthesis, Structure, and Catalytic Application" . | INORGANIC CHEMISTRY 64 . 2 (2025) : 1041-1047 . |
| APA | Yang, Guoping , Cao, Jiawei , Xiao, Yu , Hu, Qilong , Liu, Haoqi , Cao, Xiaohong et al. A Wavy Multiple Tm(III)-Containing Open Wells-Dawson Silicotungstate: Synthesis, Structure, and Catalytic Application . | INORGANIC CHEMISTRY , 2025 , 64 (2) , 1041-1047 . |
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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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Helical morphologies are widely observed in nature, however, it is very challenging to prepare artificial helical polymers. Especially, precisely understanding the structure information of artificial metal-free helical covalent inorganic polymers via single-crystal X-ray diffraction (SCXRD) analysis is rarely explored. Here, we successfully prepare a novel metal-free helical covalent inorganic polymer ({[Te(C6H5)2] [PO3(OH)]}n, named CityU-10) by introducing angular anions (HOPO32-) into traditional tellurium-oxygen chains. The dynamic reversibility of the reaction is realized through the introduction of organic tellurium precursor and the slow hydrolysis of polyphosphoric acid. High-quality and large-size single crystals of CityU-10 have been successfully characterized via SCXRD, where the same-handed helical inorganic polymer chains form a pseudo-two-dimensional layer via multiple hydrogen-bonding interactions. The left-handed layers and right-handed layers alternatively stack together through weak hydrogen bonds to form a three-dimensional supramolecular structure. The single crystals of CityU-10 are found to display promising optical properties with a large birefringence. Our results would offer new guidelines for designing and preparing new crystalline covalent polymers through tellurium-based chemistry. A metal-free helical covalent inorganic polymer (CityU-10) has been successfully prepared. Its crystal structure shows that the same-handed helical chains form a pseudo-two-dimensional layer via multiple hydrogen-bonding interactions. Then, the left-handed layers and right-handed layers alternatively stack together to form a three-dimensional supramolecular structure.image
Keyword ：
Helix Helix Inorganic Covalent Polymers Inorganic Covalent Polymers Metal-Free Structures Metal-Free Structures Optical Properties Optical Properties Single Crystals Single Crystals
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| GB/T 7714 | Xue, Miaomiao , Zhang, Lei , Wang, Xiang et al. A Metal-Free Helical Covalent Inorganic Polymer: Preparation, Crystal Structure and Optical Properties [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (6) . |
| MLA | Xue, Miaomiao et al. "A Metal-Free Helical Covalent Inorganic Polymer: Preparation, Crystal Structure and Optical Properties" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 6 (2024) . |
| APA | Xue, Miaomiao , Zhang, Lei , Wang, Xiang , Dong, Qiang , Zhu, Zengkui , Wang, Xin et al. A Metal-Free Helical Covalent Inorganic Polymer: Preparation, Crystal Structure and Optical Properties . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (6) . |
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Two inorganic-organic hybrid polyoxotantalates, H-4[Na(H2O)(5)](2)[Co-II(en)(3)](2){[Co-III(en)](2)(Ta6O19)(2)}center dot 22H(2)O (1) and H2K2Na6 (H2O)(24){[Co-III(en)](2)(Ta6O19)(2)}33H(2)O (2) have been constructed from {[Co-III(en)(Ta6O19)](2)}(10-) ({Co2Ta12}) dimers. Compound 1 has a three-dimensional supramolecular framework with a pcu-type topology. Compound 2 possesses a three-dimensional structure composed of {Co2Ta12} dimers and alkali metal ions (Na+/K+) via coordination bonds. Polyoxotantalates 1 and 2 have been used as active materials for ITO/1/Ag and ITO/2/Ag RRAM devices. These devices exhibit stable non-volatile storage behavior and rewritable resistive switching with high ON/OFF ratios of 1.43 x 10(3) and 2.17 x 10(4) for 1-based and 2-based RRAM devices, respectively, and stable cyclic performance during 100-cycle stability tests. This discovery opens up new opportunities for the development of electrical bistability materials.
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| GB/T 7714 | Cao, Yun-Fei , Lin, Yu-Jin , Li, Xin-Xiong et al. Two resistance-switchable hybrid polyoxotantalates based on {Co2Ta12} clusters [J]. | CRYSTENGCOMM , 2024 , 26 (26) : 3527-3534 . |
| MLA | Cao, Yun-Fei et al. "Two resistance-switchable hybrid polyoxotantalates based on {Co2Ta12} clusters" . | CRYSTENGCOMM 26 . 26 (2024) : 3527-3534 . |
| APA | Cao, Yun-Fei , Lin, Yu-Jin , Li, Xin-Xiong , Sun, Yan-Qiong , Zheng, Shou-Tian . Two resistance-switchable hybrid polyoxotantalates based on {Co2Ta12} clusters . | CRYSTENGCOMM , 2024 , 26 (26) , 3527-3534 . |
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Here, a case of bilayer heterojunction Pd-containing polyoxotungstate (POW), connecting a Te3Pd3 ring and an Anderson-like TeW6 cluster, has been synthesized. The Anderson-like cluster is the first example in POW. The coordination of Pd in the ring with the S atom on the sulfo group breaks the traditional coordination configuration of Pd and O in polyoxometalates (POMs), enriching the structural types of Pd-containing POMs. In addition, the hybrid bilayer heterojunction structure at the molecular level not only provides high thermal stability but also results in spatial arrangement anisotropy, leading to up to five times the anisotropic proton conductivity. © 2024 American Chemical Society.
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| GB/T 7714 | Jia, L. , Liu, Y.-X. , Li, X.-X. et al. A Palladium-Containing Polyoxotungstate with Anisotropic Proton Conductivity [J]. | Inorganic Chemistry , 2024 , 63 (31) : 14308-14312 . |
| MLA | Jia, L. et al. "A Palladium-Containing Polyoxotungstate with Anisotropic Proton Conductivity" . | Inorganic Chemistry 63 . 31 (2024) : 14308-14312 . |
| APA | Jia, L. , Liu, Y.-X. , Li, X.-X. , Sun, C. , Zheng, S.-T. . A Palladium-Containing Polyoxotungstate with Anisotropic Proton Conductivity . | Inorganic Chemistry , 2024 , 63 (31) , 14308-14312 . |
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Polyoxometalates (POMs) have good potential for applications in different fields, including conducting materials, optics, and electrocatalysis. Of particular significance is the synthesis and development of addendum POMs. Molybdenum-oxo clusters, which are renowned for their diverse structures and electronic properties, were utilized to facilitate the synthesis of innovative materials. Herein, we employed presynthesized {XW9 Nb3O40} (X= Si/Ge) polyanions as secondary building units and different molybdenum-oxo clusters as linkers. Four new addendum POMs were constructed, including two dimeric compounds Cs10[H2(SiW9Nb3O40)2(Mo2O4C2O4)]19H2O (1) and Cs8[H4(GeW9Nb3O40)2(Mo2O4C2O4)]17H2O (2), and two tetrameric compounds Cs15(NH4)[(SiW9Nb3O40)4(Mo4O6)]42H2O (3) and Cs10K5[H(GeW9Nb3O40)4(Mo4O6)]39H2O (4). Notably, this is the first report of Mo/W/Nb ternary mixed-addendum POMs. In addition, compounds 3 and 4 facilitate the transfer of protons through extended hydrogen-bonding networks with conductivity values of 1.16 x 10-2 and 7.73 x 10-3 Scm-1 at 85 degrees C and 98% relative humidity, respectively. Furthermore, no discernible decline in conductivity was noted over the course of 10 h.
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| GB/T 7714 | Chen, Si-Jie , Ge, Rui , Hong, Li-Hao et al. Assembly of Four Ternary Polyoxometalate Aggregates by Integrating Presynthesized {XW9Nb3O40} (X = Si/Ge) Units Using Molybdenum-Oxo Clusters [J]. | INORGANIC CHEMISTRY , 2024 , 64 (1) : 142-150 . |
| MLA | Chen, Si-Jie et al. "Assembly of Four Ternary Polyoxometalate Aggregates by Integrating Presynthesized {XW9Nb3O40} (X = Si/Ge) Units Using Molybdenum-Oxo Clusters" . | INORGANIC CHEMISTRY 64 . 1 (2024) : 142-150 . |
| APA | Chen, Si-Jie , Ge, Rui , Hong, Li-Hao , Sun, Yan-Qiong , Cai, Ping-Wei , Sun, Cai et al. Assembly of Four Ternary Polyoxometalate Aggregates by Integrating Presynthesized {XW9Nb3O40} (X = Si/Ge) Units Using Molybdenum-Oxo Clusters . | INORGANIC CHEMISTRY , 2024 , 64 (1) , 142-150 . |
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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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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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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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