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phosphotungstic acid immobilized on amino-functionalized TS-1 zeolite as a solid acid catalyst for the synthesis of tributyl citrate

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Chinese Journal of Chemical Engineering 2024年第6期70卷 199-210页

作者： Pei Li Bianfang Shi Junyao Shen Ran Cui Wenze Guo Ling Zhao Zhenhao Xi State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and TechnologyShanghai 200237China

The amino-functionalization of TS-1 zeolite followed by immobilization of phosphotungstic acid(HPW)was presented to prepare a strong solid acid catalyst for the synthesis of bio-based tributyl citrate from the esterification of citric acid and n-butanol.γ-Aminopropyltriethoxysilane(APTES)was first grafted on the TS-1 zeolite via the condensation reactions with surface hydroxyl groups,and subsequently the HPW was immobilized via the reaction between the amino groups and the protons from HPW-forming strong ionic *** Keggin structure of HPW and MFI topology of TS-1 zeolite were well maintained after the *** amino-functionalization generated abundant uniformly distributed active sites on TS-1 for HPW immobilization,which promoted the dispersity,abundance,as well as the stability of the acid *** tetrahedrally coordinated framework titanium and non-framework titania behaved as weak Lewis acid sites,and the protons from the immobilized HPW acted as the moderate or strong Brønsted acid *** optimized TBC yield of 96.2%(mol)with a conversion of-COOH of 98.1%(mol)was achieved at 150℃for 6 h over the HPW immobilized on amino-functionalized *** catalyst exhibited good stability after four consecutive reaction runs,where the activity leveled off at still a relatively high level after somewhat deactivation possibly caused by the leaching of a small portion of weakly anchored APTES or HPW.

关键词： Amino-functionalization phosphotungstic acid TS-1 zeolite Esterification Tributyl citrate

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Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization

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Chinese Journal of Chemical Engineering 2023年第11期63卷 140-147页

作者： Chongfu Wu Changsheng Chen Zhaoyang Qi Jie Chen Qinglian Wang Changshen Ye Ting Qiu College of Chemical Engineering Fuzhou UniversityFuzhou 350108China Qingyuan Innovation Laboratory Quanzhou 362801China Engineering Research Center of Reactive Distillation Fujian Province Higher Education InstitutesFuzhou 350108China

The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection *** desulfurization(ODS)was considered to be the most promising *** facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging *** this paper,pentamethylene hexamine(PEHA)and phosphotungstic acid(HPW)were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel *** composite material exhibited excellent catalytic activity and high recyclability,which could reach a 100% dibenzothiophene(DBT)removal rate in 30 min and be recycled at least 5 *** and DFT simulations were used to better examine the ODS mechanism of *** was proved that the rich amino groups on the surface of PEHA-HPW play a crucial *** work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.

关键词： Oxidation Catalyst Desulfurization Fuel phosphotungstic acid Amino

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Catalytic oxidative desulfurization of gasoline using phosphotungstic acid supported on MWW zeolite

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Frontiers of Chemical Science and Engineering 2020年第4期14卷 546-560页

作者： Hanlu Wang Idris Jibrin Xingye Zeng College of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming 525000China

Catalysts for the desulfurization of gasoline samples were synthesized via the immobilization of well-dispersed phosphotungstic acid(HPW)on Mobil compo-sition of matter-twenty-two(MWW)***-tion results indicated that these catalysts possess a mesoporous structure with the retention of the Keggin structure of immobilized *** reaction para-meters influencing sulfur removal were systematically investigated,including HPW loading,catalyst dosage,temperature,initial S-concentration,molar ratio of oxidant to sulfide(O/S),volume ratio of MeCN to model oil(Ext./oil),and sulfide *** 40 wt-%HPW/MWW catalyst exhibited the highest catalytic activity with 99.6%dibenzothiophene sulfur removal from prepared *** 40 wt-%HPW/MWW catalyst was recycled four times and could be easily ***,as an exploratory study,straight-run-gasoline and fluid catalytic cracking gasoline were employed to accurately evaluate the desulfurization performance of 40 wt-%HPW/*** research provides new insights into the development and application of catalysts for desulfurization of gasoline.

关键词： oxidative desulfurization phosphotungstic acid MWW wet impregnation adsorption energy

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Encapsulation of ionic liquid, phosphotungstic acid inside the nanocages of MIL-101(Cr): Effective and reusable catalyst for efficient solvent-free oxidative desulfurization from fuel oil

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Petroleum Science 2023年第6期20卷 3865-3874页

作者： Bo-Long Jiang Dong-Xu Zhang Dan-Dan Yuan Yan-Guang Chen Tian-Zhen Hao Hua Song Innovation Institute for Sustainable Maritime Architecture Research and Technology Qingdao University of TechnologyQingdao 266000ShandongChina Provincial Key Laboratory of Oil&Gas Chemical Technology College of Chemistry&Chemical EngineeringNortheast Petroleum UniversityDaqing 163318HeilongjingChina Hebei Jingzhi Technology Co. LTDCangzhou 061000HebeiChina

Oxidative desulfurization from fuel oil is one of the important methods for deep *** development of efficient oxidative desulfurization catalysts is crucial for improving the desulfurization *** encapsulation of phosphotungstic acid(HPW)and ionic liquid(BMImBr)inside the mesoporous cages of MIL-101(Cr)was accomplished through a combination of“bottle around ship”and“ship in bottle”*** obtained BMImPW@MIL-101(Cr)composite was characterized by XRD,FTIR,BET,SEM,XPS and ICP *** indicated that the BMImPW@MIL-101(Cr)composites with PW^(3−) loading of 23.1–50.7 wt%were obtained,demonstrating that the“bottle around ship”method is beneficial to make full use of nanocages of MIL-101(Cr)to obtain expected high loading of active PW^(3−) .The BMImPW@MIL-101(Cr)exhibits excellent reusability with no evidence of leaching of active PW^(3−) and BMIm^(+),and well-preserved structure after successive cycles of regeneration and *** significantly improved stability of BMImPW@MIL-101(Cr)as compared to HPW@MIL-101(Cr)is possibly because the leaching of the active PW^(3−) −sites can be greatly suppressed by forming large size of BMImPW owing to introduction of BMIm^(+)*** BMImPW@MIL-101(Cr)exhibited excellent catalytic activity for solvent free oxidative desulfurization of refractory *** enhanced oxidative desulfurization activity as compared to HPW@MIL-101(Cr)can be explained by the intimate contact of sulfides with active PW^(3−) sites owing the strong attraction of BMIm^(+)cation with the sulfides.

关键词： Metal organic frameworks phosphotungstic acid lonic liquids Stability Oxidative desulfurization

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Study on the epoxidation of olefins with H_(2)O_(2)catalyzed by biquaternary ammonium phosphotungstic acid

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Chinese Journal of Chemical Engineering 2023年第6期58卷 146-154页

作者： Zijie Zhang Qianyu Zha Ying Liu Zhibing Zhang Jia Liu Zheng Zhou School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093China

Selective epoxidation of olefins is an important field in chemical *** this work,we developed a new phosphotungstic acid catalyst{[(C_8H_(17))(CH_(3))_(2)N]_(2)(CH_(2))_(3)}_(1.5){PO_(4)[WO(O_(2))_(2)]_(4)}with long carbon chain and biquaternary ammonium *** could be epoxidized to cyclohexene oxide in 96.3%conversion and 98.2%*** catalyst type,solvent type,catalyst loading,initial molar ratio,temperature,cycle performance and substrate extensibility were studied and optimized,the kinetic parameters about overall reaction and unit reaction were also *** light scattering analysis was carried out to explain the different catalytic performance between catalysts with different carbon chain *** novel catalyst and the corresponding dynamics and mechanism study could probably help the industrial application on the epoxidation of cyclohexene with H_(2)O_(2).

关键词： Epoxidation of olefins phosphotungstic acid Cyclohexene Kinetic study

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A Direct Liquid Fuel Cell with High Power Density Using Reduced phosphotungstic acid as Redox Fuel

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Energy & Environmental Materials 2022年第1期5卷 278-284页

作者： Yiyang Liu Ting Feng Shanfu Lu Haining Wang Yan Xiang Beijing Key Laboratory of Bio-inspired Energy Materials and Devices School of Space and EnvironmentBeihang UniversityBeijing 100191China School of Energy and Power Engineering Beihang UniversityBeijing 100191China

Direct liquid fuel cells(DLFCs)are proposed to address the problems of high cost and complex storage and transportation of hydrogen in traditional hydrogen-oxygen proton exchange membrane fuel ***,present fuels of organic small molecules used in DLFCs are restricted to problems of sluggish electrochemical kinetics and easily poisoning of precious metal ***,we demonstrate reduced phosphotungstic acid as a liquid fuel for DLFCs based on its advantages of high chemical and electrochemical stability,high electrochemical activity on common carbon material electrodes,and low permeability through proton exchange *** application of phosphotungstic acid fuel effectively solves the problems of high cost of anode catalysts and serious fuel permeation loss in traditional DLFCs.A phosphotungstic acid fuel cell achieves a peak power density of466 mW cm^(-2)at a cell voltage of 0.42 V and good stability at current densities in the range from 20 to 200 mA cm^(-2).

关键词： direct liquid fuel cell heteropoly acid phosphotungstic acid power density renewable fuel

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Three-dimensionally Ordered Macroporous phosphotungstic acid/SiO2 for Efficient Catalytic Oxidative Desulfurization

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Journal of Wuhan University of Technology(Materials Science) 2018年第4期33卷 849-854页

作者：杜岳 YANG Peng 雷家珩 ZHOU Shiyu LI Junsheng DU Xiaodi School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China School of Chemistry Chemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070China

Three-dimensionally ordered（3DOM） macroporous phosphotungstic acid/SiO_2（HPW/SiO_2） materials were prepared by using colloidal crystal as templates and applied for oxidative desulfurization（ODS） of the model fuel oil. The obtained HPW/SiO_2 materials were characterized through scanning electron microscopy, powder X-ray diffraction, N_2 sorption, and Fourier transform infrared spectroscopy. The results indicated that 3 DOM HPW/SiO_2 possessed hierarchical pore architectures which contained ordered macropores and disordered mesopores, with the Keggin type HPW embedded in the framework of pore structure. The removal rate of dibenzothiophene（DBT） could reach 100% under the optimum conditions, moreover. The performance was only slightly decreased for the regenerated catalyst after 7 cycles.

关键词： three-dimensionally ordered macroporous SiO2 phosphotungstic acid oxidativedesulfurization

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Ball-milling Synthesis of Tetrahydroquinolines via 'One-pot' Three-component Diels-Alder Reaction Catalyzed by phosphotungstic acid

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Chemical Research in Chinese Universities 2020年第5期36卷 835-842页

作者： WANG Zeyou SHEN Guodong HUANG Xianqiang GONG Shuwen YANG Bingchuan SUN Zhenzhen ZHANG Zuhao LIU Wanxing School of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252000P.R.China Department of Chemistry Liaocheng Chemical Institute of Industrial ScienceLiaocheng 252000P.R.China

We reported an economic and practical ball-milling method for the synthesis of tetrahvdroquinoline derivatives via a wone-pot"three-component Diels-Alder reaction of anilines,aldehydes and alkenes catalyzed by phos-photungstic acid at room *** this reaction,a simple 'one-pot'ball-milling operation was conducted,readily available starting materials were employed,'one-pot'conditions were applied,and the most important was to use inexpensive and environmentally friendly catalyst phosphotungstic *** tetrahvdroquinolines,which might be potentially applicable in the pharmaceutical and biochemical areas,were conveniently synthesized in moderate to excellent yields.

关键词： Ball-milling Diels-Alder reaction phosphotungstic acid Tetraliydroquinoline

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Investigation of Propene Oligomerization Catalyzed by phosphotungstic acid Catalysts

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China Petroleum Processing & Petrochemical Technology 2012年第3期14卷 10-16页

作者： Liu Yinong Duan Qinghua Research Institute of Petroleum Processing SINOPEC

In this paper, the propene oligomerization reaction catalyzed by phosphotungstic acid supported on two kinds of silica gel was studied, it had been found out that the conversion of propene catalyzed by the type A silica gel-phosphotung- stic acid catalyst was 3.38 m%, while the conversion of propene catalyzed by the type B silica gel-phosphotungstic acid catalyst was 90.1 m% with a nonene selectivity of 42.33 m%, and a dodecene selectivity of 31.79 m%. The influence of reaction temperature, pressure and liquid hourly space velocity （LHSV） on the reaction catalyzed by the type B silica gel- phosphotungstic acid catalyst was investigated. It had been verified that when the reaction temperature increased from 170 ~C to 190 ~C, the conversion of propene increased while the selectivity of nonene and dodecene decreased; when the re- action pressure increased from 3.5 MPa to 4.5 MPa, the conversion of propene increased also, and the selectivity of nonene and dodecene changed very little. The conversion of propene at a space velocity of between 0.5 h-1 and 1.0 h-~ was higher than that achieved at 2.0 h-~, but the selectivity of nonene and dodecene did not show regular fluctuations. An optimum conversion of propene （91.05 m%） and an optimum selectivity of nonene and dodecene （89.51 m%） could be achieved at a reaction temperature of 170 ~C, a reaction pressure of 4.5MPa, and a LHSV of 1.0 fit. The experiments on catalyst life showed that the activity of the type B silica gel-phosphotungstic acid catalyst could be only maintained in 25 hours, and the reason was explained also.

关键词： phosphotungstic acid support propene oligomerization conversion selectivity nonene dodecene

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Synergistic Effect between Zr-MOF and phosphotungstic acid for Oxidative Desulfurization

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China Petroleum Processing & Petrochemical Technology 2020年第4期22卷 56-62页

作者： Zong Mengya Zhao Yutong Fan Cunzheng Wang Danhong TKL of Metal and Molecule Based Material Chemistry National Institute for Advanced MaterialsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350 Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071

PTA/UiO-66 composites were successfully synthesized by the hydrothermal *** results showed that the synergistic effect between phosphotungstic acid(PTA)and UiO-66 could enhance the oxidative desulfurization(ODS)*** XRD results proved that UiO-66 retained its structure in the PTA/UiO-66 *** SEM results showed that the PTA/UiO-66 catalysts exhibited regular octahedral *** Raman spectra revealed that PTA in the composites retained the Keggin *** XPS results showed that the electron transfer occurred from Zr-MOF to *** ODS reaction mechanism was *** transfer from Zr-MOF to PTA can promote the generation of active species(·OH)and thus enhance the ODS *** explanation can be confirmed by the formation of oxygen vacancy and W0 as revealed by the XPS analysis.

关键词： phosphotungstic acid Zr-MOF oxidative desulfurization synergistic effect oxygen vacancy

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