期刊
DALTON TRANSACTIONS
卷 49, 期 21, 页码 7234-7244出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0dt00217h
关键词
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资金
- National Natural Science Foundation of China [21671091, 21601077, 21773102]
- Natural Science Foundation of Liaoning Province [20180550544]
- Opening Project of Key Laboratory of Polyoxometalate Science of Ministry of Education
- Scientific Research Project of Liaoning Normal University [GD19L005]
Two new tungstosilicates (C(NH2)(3))(5)KNa2H3[Sn(CH2CH2COOCH3)Co(H2O)(2)Si2W19O69]center dot 10H(2)O (Si2W19-Co-SnRCOOCH3) and (C(NH2)(3))(5)KNa2H3[Sn(CH2CH2COOCH3)Mn(H2O)(2)Si2W19O69]center dot 13H(2)O (Si2W19-Mn-SnRCOOCH3) modified by organometal (OM) and transition metal (TM) ions were obtained, and they were self-assembled from mono-TM-containing (TM = Co, Mn)gamma-[SiW10O35](6-) (gamma-SiW10)-based dimeric tungstosilicate and estertin Cl3SnCH2CH2COOCH3 in an acetate buffer solution, respectively. Their structures were determined with a series of physico-chemical and spectroscopic methods including X-ray crystallography, XRPD, etc. The estertin functional position in the tungstosilicate skeleton was analyzed by theoretical calculations using density functional theory (DFT). These two compounds have good catalytic activity for the oxidation of cyclohexanol to cyclohexanone. Meanwhile, they were composited with TiO2 using a facial layer-by-layer (LBL) method. The assembled composite films {Si2W19-TM-SnRCOOCH3/TiO2}(n) (TM = Co, Mn; n is the bilayer number, n = 1-6) exhibit efficient photoelectrocatalytic activity for the oxidation of methanol under irradiation of 100 mW cm(-2) using a Xe lamp as a light source. And the {Si2W19-Co-SnRCOOCH3/TiO2}(4) film produces the highest photocurrent among the composite films studied in this work. Combining the dark current measurement, surface photovoltage spectroscopy (SPV) and electrochemical impedance spectroscopy (EIS), the enhanced photoelectrocatalytic activity of {Si2W19-Co-SnRCOOCH3/TiO2}(4) composite film for the oxidation of methanol is attributed to the suppressed electron-hole recombination, increased carrier separation efficiency and interfacial charge transfer.
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