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silicotungstic acid-derived WO_(3) composited with ZrO_(2) supported on SBA-15 as a highly efficient mesoporous solid acid catalyst for the alkenylation of p-xylene with phenylacetylene

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Chinese Chemical Letters 2022年第3期33卷 1325-1330页

作者： Xueting Bai Yongle Guo Zhongkui Zhao State Key Laboratory of Fine Chemicals Department of Catalysis Chemistry and EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China

Highly dispersed silicotungstic acid-derived WO_(3) composited with ZrO_(2) supported on SBA-_(15) (WZ/SBA-_(15)) as an ordered mesoporous solid acid catalyst was prepared via a facile incipient wetness impregnation (IWI) method that active ingredients, ZrO_(2) and WO_(3), were impregnated into the channels of SBA-_(15) simultaneously with a subsequent calcination process. The relationship between catalyst nature and performance was explored by high resolution transmission electron microscopy (HRTEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), FT-IR, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), N_(2) adsorption-desorption, NH_(3) temperature-programmed desorption (NH_(3)-TPD), and FT-IR of pyridine adsorption (Py-IR) characterization techniques. The catalytic performance of W_(12)Z_(15)/SBA-_(15) is not only greater than that of single component solid acid catalysts, WO_(3)/SBA-_(15) and ZrO_(2)/SBA-_(15), but also W_(12)/Z_(15)/SBA-_(15) prepared by impregnating active ingredients, ZrO_(2) and WO_(3), into SBA-_(15) in sequence. The outstanding performance of W_(12)Z_(15)/SBA-_(15) is derived from the strong interaction between ZrO_(2) and WO_(3), which results in more acid sites, and relatively high specific surface area, large pore volume, and ordered mesoporous structure of SBA-_(15). The characterization and reaction results clearly demonstrate that the synergy of ZrO_(2) and WO_(3) has a clear boost for the alkenylation. The optimized W_(12)Z_(15)/SBA-_(15)-500 achieves a 99.4% conversion of phenylacetylene and a 92.3% selectivity of main product α-arylstyrene for the alkenylation of p-xylene with phenylacetylene, with very low level of oligomers producing at the same time. Moreover, W_(12)Z_(15)/SBA-_(15)-500 shows excellent catalytic stability and regeneration. Therefore, W_(12)Z_(15)/SBA-_(15)-500 is a promising solid acid catalyst for the alkenylation.

关键词： Alkenylation SBA-15 Zirconium dioxide Tungsten trioxide silicotungstic acid Solid acid

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Efficient degradation of methyl orange via multilayer films of titanium dioxide and silicotungstic acid

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Science China Chemistry 2012年第11期55卷 2366-2372页

作者： NIU Ping HAO JingCheng Key Laboratory for Colloid and Interface Chemistry Ministry of EducationShandong UniversityJinan 250100China Key Laboratory of Coordination Chemistry and Functional Materials in Universities of Shandong Province Dezhou UniversityDezhou 253023China

We report layer-by-layer （LbL） assembly of TiO2 and H4SiW12O40 （SiW12） multilayer film on silicon wafers and glass slides for photocatalytic degradation of methyl orange （MO）. The photocatalytic efficiency of the obtained multilayer film increases along with the decrease of pH and salt concentration of the incubation solution. The results show that MO can be almost re- moved in pH 2.0 solution without salt addition in the first 60 min incubation when MO concentration is lower than 15 mg/L. Different salts show an apparent inhibitory effect on photocatalytic degradation of MO with the order of ZnC12〉KCI〉 NaC1〉LiCI. The TiO2/SiW12 multilayer film maintains photocatalytic activity even after five degradation cycles. The reaction of MO photodegradation accords with an apparent first-order dynamics.

关键词： TiO2 silicotungstic acid LbL assembly photocatalytic degradation methyl orange

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A Novel MIL-101(Cr)acidified by silicotungstic acid and Its Catalytic Performance for Isomerization of n-Heptane

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China Petroleum Processing & Petrochemical Technology 2022年第1期24卷 68-80页

作者： Zhang Wei Liu Rongjiang Ma Shoutao Kuvshinov Dimitriy Suo Yanhua Wang Yingjun Provincial Key Laboratory of College of Polyolefin New Materials Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318 Daqing Chemical Research Center of PetroChina Daqing 163714 School of Engineering University of HullUK

The 0.4%Pt/xSTA-MIL-101(Cr)metal-acid bifunctional catalysts were prepared by impregnation using STA-MIL-101(Cr)as the *** synthesized samples were verified to exhibit a typical octahedral structure of MIL-101(Cr)and the pore structure was arranged *** specific surface area of the samples was extremely high and the samples were made of micro-mesoporous composite *** acid could retain its Keggin structure in the 0.4%Pt/xSTA-MIL-101(Cr)samples and the catalyst possessed moderately strong Brønsted acid ***,the dispersion of Pt particles in MIL-101(Cr)was relatively high.n-Heptane isomerization was first used as a probe to test the novel 0.4%Pt/xSTA-MIL-10(Cr)*** with the conventional silicate catalysts,the catalytic performance of 0.4%Pt/30%STA-MIL-101(Cr)was significantly improved with a n-heptane conversion of 58.93%and an iso-heptane selectivity of 95.68%,respectively,under conditions covering a reaction time of 2 h and a reaction temperature of 260°*** catalyst could still maintain a relatively high catalytic performance after a reaction time of 5 *** with the non-noble metal catalyst,the catalytic efficiency of 0.4%Pt/30%STA-MIL-101(Cr)is relatively *** mechanism model of n-heptane isomerization over 0.4%Pt/xSTA-MIL-101(Cr)catalyst was established.

关键词： MIL-101 silicotungstic acid n-heptane isomerization platinum

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Efficient degradation of methyl orange via multilayer films of titanium dioxide and silicotungstic acid

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中国科学:化学 2012年第11期42卷 1656-1657页

作者： NIU Ping 1,2 & HAO JingCheng 1 1 Key Laboratory for Colloid and Interface Chemistry,Ministry of Education Shandong University,Jinan 250100,China 2 Key Laboratory of Coordination Chemistry and Functional Materials in Universities of Shandong Province,Dezhou University,Dezhou 253023,China Key Laboratory for Colloid and Interface Chemistry Ministry of Education Shandong University Jinan 250100 China Key Laboratory of Coordination Chemistry and Functional Materials in Universities of Shandong Province Dezhou University Dezhou 253023 China

We report layer-by-layer (LbL) assembly of TiO2 and H4SiW12O40 (SiW12) multilayer film on silicon wafers and glass slides for photocatalytic degradation of methyl orange (MO).The photocatalytic efficiency of the obtained multilayer film increases along with the decrease of pH and salt concentration of the incubation *** results show that MO can be almost removed in pH 2.0 solution without salt addition in the first 60 min incubation when MO concentration is lower than 15mg/*** salts show an apparent inhibitory effect on photocatalytic degradation of MO with the order of ZnCl2 >KCl> NaCl>*** TiO2 /SiW12 multilayer film maintains photocatalytic activity even after five degradation *** reaction of MO photodegradation accords with an apparent first-order dynamics.

关键词： TiO2 silicotungstic acid LbL assembly photocatalytic degradation methyl orange

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Study on Self-assembled Multilayer Film Formed by a Binuclear Ruthenium Complex and silicotungstic acid

Study on Self-assembled Multilayer Film Formed by a Binuclea...

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中国化学会第十届全国无机化学学术会议

作者： Yin hongju Yu ying Cheng feixiang He chixian Yang yuting Liu zining Qujing Normal University

A new self-assembled multiplayer film was successfully prepared by alternating adsorption of a binuclear ruthenium complex [RuL(bpy)] and silicotungstic acid. The film was characterized by means of UV-visible absorpti... 详细信息

关键词： Binuclear Ruthenium Complex Self-assembled film silicotungstic acid

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H_(4)SiW_(12)O_(40)-catalyzed cyclization of epoxides/aldehydes and sulfonyl hydrazides: An efficient synthesis of 3,4-disubstituted 1H-pyrazoles

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Chinese Chemical Letters 2022年第3期33卷 1483-1487页

作者： Guoping Yang Xuanjie Xie Mengyuan Cheng Xiaofei Gao Xiaoling Lin Ke Li Yuanyuan Cheng Yufeng Liu Jiangxi Key Laboratory for Mass Spectrometry and Instrumentation Jiangxi Province Key Laboratory of Synthetic ChemistryEast China University of TechnologyNanchang 330013China Henan Key Laboratory of Polyoxometalate Chemistry College of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004China

A simple and efficient method for the synthesis of pyrazoles through a silicotungstic acid (H_(4)SiW_(12)O_(40))-catalyzed cyclization of epoxides/aldehydes and sulfonyl hydrazides has been developed. Various epoxides/aldehydes were smoothly reacted with sulfonyl hydrazides to furnish regioselectivity 3,4-disubstituted 1H-pyrazoles. The application of such an earth-abundant, readily accessible, and nontoxic catalyst provides a green approach for the construction of 3,4-disubstituted 1H-pyrazoles. A plausible reaction mechanism has been proposed on the basis of control experiments, GC-MS and DFT calculations.

关键词： silicotungstic acid Epoxides Aldehydes Sulfonyl hydrazides 3,4-Disubstituted 1H-pyrazoles

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Synthesis and Crystal Structure of a Novel 1D Chain-like Organic Inorganic Hybrid Rare Earth Derivative of Polyoxometalate: H_(0.5)[Sm(H_2O)_6]_(0.25)[Sm(H_2O)_5]_(0.25){[Sm(H_2O)_7][Sm(H_2O)_2-(DMSO)][SiW_(11)O_(39)]}·4.5H_2O

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Chinese Chemical Letters 2005年第12期16卷 1655-1658页

作者： Jun Wei ZHAO Jing Ping WANG Jing Yang NIU School of Chemistry and Chemical Engineering Henan University Kaifeng 475001

A 1D chain-like organic-inorganic hybrid rare earth derivative of polyoxometalate H0.5[Sm（H2O）6]0.25[Sm（H2O）5]0.25{[Sm（H2O）7][Sm（H2O）2（DMSO）][SiW11O39]}·4.5H2O has been firstly synthesized by reaction of α-K8SiW11O39.13H2O, HClO4, Sm2O3 with dimethyl sulfoxide （DMSO） and characterized by elemental analysis, IR spectra and single crystal X-ray diffraction. The neighboring polyanionic units {[Sm（H2O）7][Sm（H2O）2（DMSO）][SiWHO39]}^2- are bridged together to a 1D chain structure by means of [Sm（H2O）2（DMSO）]^3＋ ion.

关键词： silicotungstic acid polyoxometalate mono-vacant Keggin structure rare earth ions

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Synthesis, characterization and catalytic application of H4SiW12O40/MCM-48 in the esterification of methacrylic acid with n-butyl alcohol

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Journal of Chemistry and Chemical Engineering 2009年第1期3卷 61-65页

作者： YANG Shui-jin YIN Guo-jun ZHANG Yi-jun WANG Dong-ming Hubei Key Laboratory of Pollutant Analysis ＆ Reuse Technology College of Chemistry and Environmental Engineering Hubei Normal University Huangshi 435002 China

A novel environmental friendly catalyst, H4SiW12O40/MCM-48, was prepared by impregnation method. The catalysts were characterized by means of XRD and FT-IR. The synthesis of n-butyl methacrylate catalyzed by H4SiW12O40/MCM-48 was studied with methacrylic acid and n-butyl alcohol as reactants. H4SiW12O40/MCM-48 was an excellent catalyst for the synthesis of n-butyl methacrylate and Keggin structure ofH4SiW12O40 kept unchanged after impregnated on surface of the molecular sieve support. Effects of n（methacrylic acid）： n（n-butyl alcohol）, catalyst dosage, cyclohexane （water-stripped reagent） and reaction time on the yields of the product were investigated. The optimum conditions have been found, that is, molar ratio of acid to alcohol is 1：1.5, mass ratio of catalyst used to the reactant is 1.5%, cyclohexane is 10 mL and reaction time is 1.5h. Under these conditions, the yield of n-butyl methacrylate can reach 73.2%.

关键词： MCM-48 molecular sieve silicotungstic acid n-butyl methacrylate catalysis

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