A variety of spherical and structured activated charcoal supported Pt/Fe3O4 composites with an average particle size of ~100 nm have been synthesized by a self-assembly method using the difference of reduction potenti...A variety of spherical and structured activated charcoal supported Pt/Fe3O4 composites with an average particle size of ~100 nm have been synthesized by a self-assembly method using the difference of reduction potential between Pt (Ⅳ) and Fe (Ⅱ) precursors as driving force. The formed Fe3O4 nanoparticles (NPs) effectively prevent the aggregation of Pt nanocrystallites and promote the dispersion of Pt NPs on the surface of catalyst, which will be favorable for the exposure of Pt active sites for high-efficient adsorption and contact of substrate and hydrogen donor. The electron-enrichment state of Pt NPs donated by Fe304 nanocrystallites is corroborated by XPS measurement, which is responsible for promoting and activating the terminal C=O bond of adsorbed substrate via a vertical configuration. The experimental results show that the activated charcoal supported Pt/Fe3O4 catalyst exhibits 94.8% selectivity towards cinnamyl alcohol by the transfer hydrogenation of einnamaldehyde with Pt loading of 2.46% under the optimum conditions of 120 ℃ for 6 h, and 2-propanol as a hydrogen donor. Additionally, the present study demonstrates that a high-efficient and recyclable catalyst can be rapidly separated from the mixture due to its natural magnetism upon the application of magnetic field.展开更多
Pt/FeSnO(OH)_5 was synthesized as a novel catalyst for VOCs oxidation. Compared with Pt/γ-Al_2O_3 during catalytic oxidation of benzene, Pt/Fe Sn O(OH)5 showed better catalytic activity. After characterization of...Pt/FeSnO(OH)_5 was synthesized as a novel catalyst for VOCs oxidation. Compared with Pt/γ-Al_2O_3 during catalytic oxidation of benzene, Pt/Fe Sn O(OH)5 showed better catalytic activity. After characterization of the catalysts by XRD, SEM, TEM, EDS, XPS, BET, TGA and DTA, we found most Pt could be reduced to metallic state when the hydroxyl catalyst was used as supporter, and the metallic Pt in Pt/Fe Sn O(OH)5 was more active than the oxidized Pt in Pt/γ-Al_2O_3 in catalytic oxidation of VOCs. Pt/FeSnO(OH)_5 shows both good catalytic activity and high stability, which may be a promising catalyst. This study may also be helpful for the design and fabrication of new catalysts.展开更多
An efficient and low-cost supported Pt catalyst for hydrogenation of niroarenes was prepared with colloid Pt precursors andα-Fe2O3 as a support.The catalyst with Pt content as low as 0.2 wt%exhibits high activities,c...An efficient and low-cost supported Pt catalyst for hydrogenation of niroarenes was prepared with colloid Pt precursors andα-Fe2O3 as a support.The catalyst with Pt content as low as 0.2 wt%exhibits high activities,chemoselectivities and stability in the hydrogenation of nitrobenzene and a variety of niroarenes.The conversion of nitrobenzene can reach 3170 molconv h^–1 molPt^–1 under mild conditions(30°C,5 bar),which is much higher than that of commercial Pt/C catalyst and many reported catalysts under similar reaction conditions.The spatial separation of the active sites for H2 dissociation and hydrogenation should be responsible for the high chemoselectivity,which decreases the contact possibility between the reducible groups of nitroarenes and Pt nanoparticles.The unique surface properties ofα-Fe2O3 play an important role in the reaction process.It provides active sites for hydrogen spillover and reactant adsorption,and ultimately completes the hydrogenation of the nitro group on the catalyst surface.展开更多
Ultrastable Y zeolite(USY)-supported Pt catalyst was prepared by gas-bubbling-assisted membrane reduction. The influence of reaction conditions and the metal and acid sites of catalysts on the catalytic performance ...Ultrastable Y zeolite(USY)-supported Pt catalyst was prepared by gas-bubbling-assisted membrane reduction. The influence of reaction conditions and the metal and acid sites of catalysts on the catalytic performance of catalyst in hydrogenation and selective ring opening of tetralin, 1,2,3,4-tetrahydronaphthalene(THN), was studied. It was found that the optimal reaction conditions were at a temperature of 280 °C, hydrogen pressure of 4 MPa, liquid hourly space velocity of 2 h^-1 and H2/THN ratio of 750. Under these optimal conditions, a high conversion of almost 100% was achieved on the 0.3 Pt/USY catalyst. XRD patterns and TEM images revealed that Pt particles were highly dispersed on the USY, favorable to the hydrogenation reaction of tetralin. Ammonia temperature-programmed desorption and Py-IR results indicated that the introduction of Pt can reduce the acid sites of USY, particularly the strong acid sites of USY. Thus, the hydrocracking reaction can be suppressed.展开更多
Mesoporous Co3 O4(meso-Co3 O4)-supported Pt(0.53 wt.%Pt/meso-Co304)was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO)was fabricated through in situ r...Mesoporous Co3 O4(meso-Co3 O4)-supported Pt(0.53 wt.%Pt/meso-Co304)was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO)was fabricated through in situ reduction of meso-Co304 with glycerol,and the 0.18-0.69 wt.%Pt/meso-CoO samples were generated by the PVA-assisted reduction method.Meso-Co3 O4 and meso-CoO were of cubic crystal structure and the Pt nanoparticles(NPs)with a uniform size of ca.2 nm were well distributed on the mesoCo3 O4 or meso-CoO surface.The 0.56 wt%Pt/meso-CoO(0.56 Pt/meso-CoO)sample performed the best in benzene combustion(T50%=156℃and T90%=186℃at a space velocity of 80,000 mL/(g h)).Introducing water vapor or C02 with a certain concentration led to partial deactivation of 0.56 Pt/meso-CoO and such a deactivation was reversible.We think that the superior catalytic activity of 0.56 Pt/meso-CoO was intimately related to its good oxygen activation and benzene adsorption ability.展开更多
基金This work is supported by the National Natural Science Foundation of China (No.51372248, No.51432009 and No.51502297), Instrument Developing Project of the Chinese Academy of Sciences (No.yz201421), the CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China.
文摘A variety of spherical and structured activated charcoal supported Pt/Fe3O4 composites with an average particle size of ~100 nm have been synthesized by a self-assembly method using the difference of reduction potential between Pt (Ⅳ) and Fe (Ⅱ) precursors as driving force. The formed Fe3O4 nanoparticles (NPs) effectively prevent the aggregation of Pt nanocrystallites and promote the dispersion of Pt NPs on the surface of catalyst, which will be favorable for the exposure of Pt active sites for high-efficient adsorption and contact of substrate and hydrogen donor. The electron-enrichment state of Pt NPs donated by Fe304 nanocrystallites is corroborated by XPS measurement, which is responsible for promoting and activating the terminal C=O bond of adsorbed substrate via a vertical configuration. The experimental results show that the activated charcoal supported Pt/Fe3O4 catalyst exhibits 94.8% selectivity towards cinnamyl alcohol by the transfer hydrogenation of einnamaldehyde with Pt loading of 2.46% under the optimum conditions of 120 ℃ for 6 h, and 2-propanol as a hydrogen donor. Additionally, the present study demonstrates that a high-efficient and recyclable catalyst can be rapidly separated from the mixture due to its natural magnetism upon the application of magnetic field.
基金supported by the National Natural Science Foundation of China(No.51102047,51472050)the Natural Science Foundation of Fujian Province(No.2013J05027)the Fujian Province Education-science Project for Middle-aged and Young Teachers(No.JA13050)
文摘Pt/FeSnO(OH)_5 was synthesized as a novel catalyst for VOCs oxidation. Compared with Pt/γ-Al_2O_3 during catalytic oxidation of benzene, Pt/Fe Sn O(OH)5 showed better catalytic activity. After characterization of the catalysts by XRD, SEM, TEM, EDS, XPS, BET, TGA and DTA, we found most Pt could be reduced to metallic state when the hydroxyl catalyst was used as supporter, and the metallic Pt in Pt/Fe Sn O(OH)5 was more active than the oxidized Pt in Pt/γ-Al_2O_3 in catalytic oxidation of VOCs. Pt/FeSnO(OH)_5 shows both good catalytic activity and high stability, which may be a promising catalyst. This study may also be helpful for the design and fabrication of new catalysts.
基金supported by the National Natural Science Foundation of China(21473073,21473074)‘‘13th Five-Year’’ Science and Technology Research of the Education Department of Jilin Province(2016403)+1 种基金the Development Project of Science and Technology of Jilin Province(20170101171JC,20180201068SF)the Open Project of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry(201703)~~
文摘An efficient and low-cost supported Pt catalyst for hydrogenation of niroarenes was prepared with colloid Pt precursors andα-Fe2O3 as a support.The catalyst with Pt content as low as 0.2 wt%exhibits high activities,chemoselectivities and stability in the hydrogenation of nitrobenzene and a variety of niroarenes.The conversion of nitrobenzene can reach 3170 molconv h^–1 molPt^–1 under mild conditions(30°C,5 bar),which is much higher than that of commercial Pt/C catalyst and many reported catalysts under similar reaction conditions.The spatial separation of the active sites for H2 dissociation and hydrogenation should be responsible for the high chemoselectivity,which decreases the contact possibility between the reducible groups of nitroarenes and Pt nanoparticles.The unique surface properties ofα-Fe2O3 play an important role in the reaction process.It provides active sites for hydrogen spillover and reactant adsorption,and ultimately completes the hydrogenation of the nitro group on the catalyst surface.
基金the National Natural Science Foundation of China (U1662103 and 21673290)the National HiTech Research and Development Program (863) of China (2015AA034603)the China National Offshore Oil Corporation Fund (LHYJYKJSA20160002)
文摘Ultrastable Y zeolite(USY)-supported Pt catalyst was prepared by gas-bubbling-assisted membrane reduction. The influence of reaction conditions and the metal and acid sites of catalysts on the catalytic performance of catalyst in hydrogenation and selective ring opening of tetralin, 1,2,3,4-tetrahydronaphthalene(THN), was studied. It was found that the optimal reaction conditions were at a temperature of 280 °C, hydrogen pressure of 4 MPa, liquid hourly space velocity of 2 h^-1 and H2/THN ratio of 750. Under these optimal conditions, a high conversion of almost 100% was achieved on the 0.3 Pt/USY catalyst. XRD patterns and TEM images revealed that Pt particles were highly dispersed on the USY, favorable to the hydrogenation reaction of tetralin. Ammonia temperature-programmed desorption and Py-IR results indicated that the introduction of Pt can reduce the acid sites of USY, particularly the strong acid sites of USY. Thus, the hydrocracking reaction can be suppressed.
基金supported by the National Natural Science Foundation of China(Nos.21677004,21876006,21607005,21622701,21477005,and U1507108)National Natural Science Foundation of China-Liaoning Provincial People’s Government Joint Fund(U1908204)Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)
文摘Mesoporous Co3 O4(meso-Co3 O4)-supported Pt(0.53 wt.%Pt/meso-Co304)was synthesized via the KIT-6-templating and polyvinyl alcohol(PVA)-assisted reduction routes.Mesoporous CoO(meso-CoO)was fabricated through in situ reduction of meso-Co304 with glycerol,and the 0.18-0.69 wt.%Pt/meso-CoO samples were generated by the PVA-assisted reduction method.Meso-Co3 O4 and meso-CoO were of cubic crystal structure and the Pt nanoparticles(NPs)with a uniform size of ca.2 nm were well distributed on the mesoCo3 O4 or meso-CoO surface.The 0.56 wt%Pt/meso-CoO(0.56 Pt/meso-CoO)sample performed the best in benzene combustion(T50%=156℃and T90%=186℃at a space velocity of 80,000 mL/(g h)).Introducing water vapor or C02 with a certain concentration led to partial deactivation of 0.56 Pt/meso-CoO and such a deactivation was reversible.We think that the superior catalytic activity of 0.56 Pt/meso-CoO was intimately related to its good oxygen activation and benzene adsorption ability.