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学者姓名：郑寿添
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Abstract ：
Three new group IIIA metal phosphate-oxalate (MPO) compounds, namely [(CH3)2NH2]2[M2(HPO4)2(H2PO4)2(C2O4)] (M = Al (1), Ga (2)) and [(CH3)2NH2]2[In2(HPO4)2(H2PO4)2(C2O4)]center dot H2O (3), have been synthesized. Their crystal structures feature an anionic layer with the sql topology net. In particular, 1 displays a proton conductivity (sigma) of 9.09 x 10-3 S cm-1 at 85 degrees C and under 98% relative humidity, which is the highest among MPOs. This study not only endows the main group metal-based MPO family with new members, but also contributes to further understanding of the structure-directing roles of amines and provides a feasible idea for improving the proton conductivity of MPOs. Three new layered metal phosphate-oxalates [(CH3)2NH2]2[M2(HPO4)2(H2PO4)2(C2O4)]center dot xH2O (M = Al, Ga, In) have been synthesized. [(CH3)2NH2]2[Al2(HPO4)2(H2PO4)2(C2O4)] displays the highest proton conductivity among metal phosphate-oxalates so far.
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| GB/T 7714 | Pan, Tian-Yu , Wen, Wei-Yang , Ma, Wen et al. New group IIIA metal phosphate-oxalates containing dimethylammonium cations with proton conductivity [J]. | DALTON TRANSACTIONS , 2024 , 53 (5) : 2318-2323 . |
| MLA | Pan, Tian-Yu et al. "New group IIIA metal phosphate-oxalates containing dimethylammonium cations with proton conductivity" . | DALTON TRANSACTIONS 53 . 5 (2024) : 2318-2323 . |
| APA | Pan, Tian-Yu , Wen, Wei-Yang , Ma, Wen , Zheng, Shou-Tian , Feng, Mei-Ling , Huang, Xiao-Ying . New group IIIA metal phosphate-oxalates containing dimethylammonium cations with proton conductivity . | DALTON TRANSACTIONS , 2024 , 53 (5) , 2318-2323 . |
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Atomically precise metal clusters serve as a unique model for unraveling the intricate mechanism of the catalytic reaction and exploring the complex relationship between structure and activity. Herein, three series of water-soluble heterometallic clusters LnCu(6), abbreviated as LnCu(6)-AC (Ln=La, Nd, Gd, Er, Yb; HAC=acetic acid), LnCu(6)-IM (Ln=La and Nd; IM=Imidazole), and LnCu(6)-IDA (Ln=Nd; H2IDA=Iminodiacetic acid) are presented, each featuring a uniform metallic core stabilized by distinct protected ligands. Crystal structure analysis reveals a triangular prism topology formed by six Cu(2+)ions around one Ln(3+)ion in LnCu(6), with variations in CuCu distances attributed to different ligands. Electrocatalytic oxygen evolution reaction (OER) shows that these different LnCu6clustersexhibit different OER activities with remarkable turnover frequency of 135 s(-1)for NdCu6-AC, 79 s(-1)for NdCu6-IM and 32 s(-1)for NdCu6-IDA. Structural analysis and Density Functional Theory (DFT) calculations underscore the correlation between shorter CuCu distances and improves OER catalytic activity, emphasizing the pivotal role of active-site distance in regulating electrocatalytic OER activities. These results provide valuable insights into the OER mechanism and contribute to the design of efficient homogeneous OER electrocatalysts.
Keyword ：
active-site distance active-site distance clusters clusters homogeneous catalytic homogeneous catalytic molecular catalysis molecular catalysis water oxidation water oxidation
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| GB/T 7714 | Chen, Jia-Nan , Pan, Zhong-Hua , Sun, Fu-Li et al. Tuning Electrocatalytic Water Oxidation Activity: Insights from the Active-Site Distance in LnCu6 Clusters [J]. | SMALL , 2024 , 20 (32) . |
| MLA | Chen, Jia-Nan et al. "Tuning Electrocatalytic Water Oxidation Activity: Insights from the Active-Site Distance in LnCu6 Clusters" . | SMALL 20 . 32 (2024) . |
| APA | Chen, Jia-Nan , Pan, Zhong-Hua , Sun, Fu-Li , Wu, Ping-Xin , Zheng, Shou-Tian , Zhuang, Gui-Lin et al. Tuning Electrocatalytic Water Oxidation Activity: Insights from the Active-Site Distance in LnCu6 Clusters . | SMALL , 2024 , 20 (32) . |
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A 3D tellurium-substituted heteropolyoxoniobate framework H5K3Na[Cu(en)(2)](2)[Cu(en)(0.75)(H2O)(2.5)]{[(Te2Nb19O58)(mu(3)-OH)(2)]}24H(2)O (1, en = ethylenediamine) with a 6-connected pcu topology is built from heart-shaped {Te2Nb19O60} clusters and copper complexes. The {Te2Nb19O60} cluster represents the new tellurniobate structure type with a 19-nuclearity Nb cluster. It consists of two new monovacant Lindqvist {Nb5O19} clusters, one boat-shaped {Nb9O32} cluster and two TeO32- anions. The {Te2Nb19O60} polyanions are interlinked by [Cu(en)(2)](2+) complexes into a 2D (4, 4) grid-like layer containing rhombic sheets. The Cu2+ supports the adjacent layers through Te-O-Cu-O-Te- bonds to form a three-dimensional heteropolyoxoniobate framework with 1D channels. This compound exhibits good chemical and solvent stability and proton conductivity, with a conductivity of 7.9 x 10(-3) S cm(-1) at 85 degrees C under 98% RH.
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| GB/T 7714 | Wu, Ping-Xin , Han, Yue , Lin, Yu-Jin et al. A 3D heteropolyoxoniobate framework based on heart-shaped {Te2Nb19O60} clusters with proton conductivity property [J]. | DALTON TRANSACTIONS , 2024 , 53 (17) : 7424-7429 . |
| MLA | Wu, Ping-Xin et al. "A 3D heteropolyoxoniobate framework based on heart-shaped {Te2Nb19O60} clusters with proton conductivity property" . | DALTON TRANSACTIONS 53 . 17 (2024) : 7424-7429 . |
| APA | Wu, Ping-Xin , Han, Yue , Lin, Yu-Jin , Sun, Yan-Qiong , Zheng, Shou-Tian . A 3D heteropolyoxoniobate framework based on heart-shaped {Te2Nb19O60} clusters with proton conductivity property . | DALTON TRANSACTIONS , 2024 , 53 (17) , 7424-7429 . |
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A series of proof-of-concept models of polyoxomolybdates with different protonated disubstituted aniline counterions and the same beta-Mo8O26 polyanion were synthesized to study the mechanism governing the formation of the intermolecular charge transfer (inter-CT) band. A series of proof-of-concept models of polyoxomolybdates were synthesized to study the mechanism governing the formation of the intermolecular charge transfer band.
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| GB/T 7714 | Zhang, Xiao-Yue , Fan, Jin-Ai , Chen, Zhe-Hong et al. The mechanism governing the formation of intermolecular charge transfer bands: a series of polyoxomolybdates as a case study [J]. | DALTON TRANSACTIONS , 2024 , 53 (14) : 6162-6167 . |
| MLA | Zhang, Xiao-Yue et al. "The mechanism governing the formation of intermolecular charge transfer bands: a series of polyoxomolybdates as a case study" . | DALTON TRANSACTIONS 53 . 14 (2024) : 6162-6167 . |
| APA | Zhang, Xiao-Yue , Fan, Jin-Ai , Chen, Zhe-Hong , Sun, Cai , Zheng, Shou-Tian . The mechanism governing the formation of intermolecular charge transfer bands: a series of polyoxomolybdates as a case study . | DALTON TRANSACTIONS , 2024 , 53 (14) , 6162-6167 . |
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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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A rare all-inorganic high-nuclearity mixed-valent {Mn11} cluster embedded polyoxoniobate, K25H43{(Te4Nb9O33)3(Nb6O19)5(TeVINb5O14)[(TeIVO3)2(MnII7MnIII4O19)]}·97H2O (1), has been synthesized by a one-pot reaction. Compound 1 contains the largest manganese cluster {Mn11} core among polyoxoniobates reported to date. {Mn11} consists of three quasi-cubane {Mn3O4} units and is simultaneously encapsulated by lacunary α-Keggin {Te4Nb9O36} and Lindqvist {Nb6O19} units. Compound 1 exhibits significant magnetic anisotropy and excellent water solubility and stability. The findings suggest a new, all-inorganic polynulear Mn-based structural paradigm for aqueous solution chemistry and magnetic materials. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Wu, P.-X. , Chen, C.-X. , Sun, Y.-Q. et al. A water-soluble mixed-valent {Mn11} cluster embedded heteropolyoxoniobate with magnetic properties [J]. | Chemical Communications , 2024 , 60 (67) : 8888-8891 . |
| MLA | Wu, P.-X. et al. "A water-soluble mixed-valent {Mn11} cluster embedded heteropolyoxoniobate with magnetic properties" . | Chemical Communications 60 . 67 (2024) : 8888-8891 . |
| APA | Wu, P.-X. , Chen, C.-X. , Sun, Y.-Q. , Zheng, S.-T. . A water-soluble mixed-valent {Mn11} cluster embedded heteropolyoxoniobate with magnetic properties . | Chemical Communications , 2024 , 60 (67) , 8888-8891 . |
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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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