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Multicomponent Cooperative Assembly of Nanoscale Boron-Rich Polyoxotungstates with 22 and 30 Boron Atoms

CCS Chemistry 2022年第4期4卷 1305-1314页

作者： Yi Chen Zheng-Wei Guo Xin-Xiong Li Shou-Tian Zheng Guo-Yu Yang State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhouFujian 350108 MOE Key Lab of Cluster Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488

This work demonstrates that the introduction of positive lanthanide(Ln)and transition metal(TM)cations into Polyoxotungstates(POTs)to stabilize negative oxoboron clusters is a feasible and general synthetic strategy for creating not only rare boron-rich POTs but also intriguing multicomponent composite polyoxometalates(POMs).By this strategy,a large family of unprecedented boron-rich POTs with 22 and 30 boron atoms,such as[(B_(18)Si_(3)Ln_(6)O_(36)(OH)_(14)){B_(4)Ni_(4)O_(10)(OH)_(4)(A-α-SiW_(9)O_(34))}_(3)]^(44−)(1Ln),[(B_(19)Si_(2)Ln_(7)O_(35)(OH)_(15)(H_(2)O)){B_(4)Ni_(4)O_(10)(OH)_(4)(A-α-SiW_(9)O_(34))}_(2){B_(3)Ni_(4)O_(9)(OH)_(3)(A-α-SiW_(9)-O_(34))}]^(41−)(2Ln),where Ln is Gd,Tb,and Dy,and[(B_(22)O_(42)){LnNi_(3)(OH)_(3)(B-α-SiW_(9)O_(34))}_(4)]^(34−)(3Ln;Ln is Sm,Gd,and Tb),have been obtained.These POTs incorporate the largest number of boron atoms and the highest-nuclearity oxoboron clusters of any molecular POTs reported to date.The results show the fusion of two distinct research areas of POT chemistry and oxoboron cluster chemistry.In addition,they also show a family of unique POMs made from multiple oxo clusters including W-O,B-O,TM-O,and Ln-O.Experiments indicate these novel composite materials can exhibit effective catalytic activity for oxidizing toxic 2-chloroethyl ethyl sulfide.

关键词： Polyoxotungstates multicomponent boron lanthanide transition metal

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Photocatalytic Hydrogen Evolution of Keggin-type Polyoxo-tungstates and their Electrochemical Behaviors

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Chinese Chemical Letters 2006年第7期17卷 973-976页

作者： Li Qin DANG Wan Sheng YOU Xin ZHANG Cui Ying HUANG Zhi Bin LEI Zhen Gang SUN Can LI Institute of Chemistry for Functionalized Materials Faculty of Chemistry and Chemical Engneering Liaoning Normal University Liaoning 116029 State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Science Liaoning 116023

The photocatalytic hydrogen evolution and electrochemical behaviors of Kiggen-type XW12O40^n- （X=P, Ge and Si） are investigated. It is found that the two-electron reduced species are active for H^＋ reduction and the more negative the potential of XW12O40^（n＋2）-/（n＋1）- is, the higher the activity for hydrogen evolution is.

关键词： Polyoxotungstates photocatalysis hydrogen evolution electrochemistry.

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Effect of Na(Ⅰ)-H2O clusters on self-assembly of sandwich-type U(Ⅵ)-containing silicotungstates and the efficient catalytic activity for the synthesis of substituted phenylsulfonyl-1H-pyrazoles

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Tungsten 2022年第2期4卷 149-157页

作者： Ke Li Xiao-Ling Lin Kai Zeng Xiao-Fei Gao Wei Cen Yu-Feng Liu Guo-Ping Yang Jiangxi Key Laboratory for Mass Spectrometry and Instrumentation Jiangxi Province Key Laboratory of Synthetic ChemistryEast China University of TechnologyNanchang330013China Russia School of Social and Human Sciences-International Relations Tyumen State UniversityTyumen625003Russia

In this study,a sandwich-type uranium(Ⅵ)-containing silicotungstate KNa11H2(H2O)30[Na(UO2)(SiW9O34)]2·8H2O(1)with new three-dimensional(3D)structure was synthesized and characterized using single-crystal X-ray diffraction,Fourier transform infrared,Raman,solid-state ultraviolet–visible diffuse reflection spectra,thermogravimetric analysis and powder X-ray diffraction.Single crystal analysis revealed that the Na(I)-H2O clusters in 1 showed a two-dimensional structure similar to(4,4)-network and resulted in the formation of a new 3D structure of 1.In addition,it was notable that 1 presented excellent catalytic activity for the synthesis of substituted phenylsulfonyl-1H-pyrazoles via the cyclization reaction of 1,3-diketones with various substituted benzenesulfonyl hydrazides.

关键词： Uranium Polyoxotungstates Condensation reaction Phenylsulfonyl-1H-pyrazoles

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