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
separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase, Here, core-shell Fe3O4@UiO-66-NH2 nanohybrids with well-defined structures were constructed b...separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase, Here, core-shell Fe3O4@UiO-66-NH2 nanohybrids with well-defined structures were constructed by dispersing magnets in a dimethylformamide （DMF） solution con- taining two metal-organic framework （MOF） precursors, namely ZrCI4 and 2-aminobenzenetricar- boxylic acid. This method is simpler and more efficient than previously reported step-by-step method in which magnets were consecutively dispersed in DMF solutions each containing one MOF precursor, and the obtained Fe304@UiO-66-NH2 with three assembly cycles has a higher degree of crystallinity and porosiW. The core-shell Fe3O4@UiO-66-NH2 is highly active and selective in Knoevenagel condensations because of the bifunctionality of UiO-66-NH2 and better mass transfer in the nano-sized shells. It also has good recycling stability, and can be recovered magnetically and reused at least four times without significant loss of catalytic activity and framework integrity. The effects of substitution on the reactivity of benzaldehyde and of substrate size were also investigated.展开更多
Nano TiO2/Fe3O4 composite particles with different molar ratios of TiO2 to Fe3O4 were prepared via sol-gel method. X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry were used to ch...Nano TiO2/Fe3O4 composite particles with different molar ratios of TiO2 to Fe3O4 were prepared via sol-gel method. X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry were used to characterize the TiO2/Fe3O4 particles. The photocatalytic activity of the particles was tested by degrading methyl blue solution under UV illumination （254 nm）. The results indicate that with the content of TiO2 increasing, the photocatalytic activity of the composite particles enhances, while the magnetism of the particles decreases. When the molar ratio of TiO2 to Fe3O4 is about 8, both the photocatalytic activity and magnetism of the TiO2/Fe3O4 particles are relatively high, and their photocatalytic activity remains well after repeated use.展开更多
Several catalysts comprising Pt supported on octahedral Fe3O4（Pt/Fe3O4） were prepared by a facile method involving co-precipitation followed by thermal treatment at different temperatures. A variety of characterizat...Several catalysts comprising Pt supported on octahedral Fe3O4（Pt/Fe3O4） were prepared by a facile method involving co-precipitation followed by thermal treatment at different temperatures. A variety of characterization results revealed that this preparation process afforded highly crystalline octahedral Fe3O4 with a uniform distribution of Pt nanoparticles on its surface. The thermal-treatment temperature significantly influenced the redox properties of the Pt/Fe3O4 catalysts. All the Pt/Fe3O4 catalysts were found to be catalytically active and stable for the oxidation of low-concentration formaldehyde（HCHO） with oxygen. The catalyst prepared by thermal treatment at 80 °C（labelled Pt/Fe3O4-80） exhibited the highest catalytic activity, efficiently converting HCHO to CO2 and H2 O under ambient temperature and moisture conditions. The excellent performance of Pt/Fe3O4-80 was mainly attributed to beneficial interactions between the Pt and Fe species that result in the formation a higher density of active interface sites（e.g., Pt-O-FeO x and Pt-OH-FeO x）. The introduction of water vapor improves the catalytic activity of the Pt/Fe3O4 catalysts as it participates in a water-assisted dissociation process.展开更多
Biodiesel is a green fuel which can replace diesel while addressing various issues such as scarcity of hydrocarbon fuels and environmental pollution to an extent. The high production cost of biodiesel and the recovery...Biodiesel is a green fuel which can replace diesel while addressing various issues such as scarcity of hydrocarbon fuels and environmental pollution to an extent. The high production cost of biodiesel and the recovery of the catalyst after the transesterification process are the major challenges to be addressed in biodiesel production. In the present work, a cheap and promising solid base oxide catalyst was synthesized from chicken eggshell by calcination at 900 ℃ forming catalyst eggshells(CES) and was impregnated with the nanomagnetic material(Fe3O4) to obtain Fe3O4 loaded catalytic eggshell(CES–Fe3O4). Fe3O4 nanomaterials were synthesized by co-precipitation method and were loaded in catalytic eggshell by sonication, for better recovery of the catalyst after transesterification process. CES–Fe3O4 material was characterized by Thermogravimetric analysis, X-ray diffraction, Fourier transform infrared spectroscopy, a vibrating-sample magnetometer, Brunauer-Emmett-Teller, Dynamic light scattering, and Scanning electron microscopy. Biodiesel was synthesized by transesterification of Pongamia pinnata raw oil with 1:12 oil to methanol molar ratio and 2 wt% catalyst loading for 2 h at a temperature of 65 ℃ and yields were compared. The reusability of the catalyst was studied by the transesterification of the raw oil and its catalytic activity was found to be retained up to 7 cycles with a yield of 98%.展开更多
Fe（HSO4）3 has been used as an efficient and recyclable catalyst for the one-pot synthesis of 14-aryl- or alkyl-14Hdibenzo[aj]xanthene derivatives by the reaction of 2-naphtol and aldehydes. Different types of aromat...Fe（HSO4）3 has been used as an efficient and recyclable catalyst for the one-pot synthesis of 14-aryl- or alkyl-14Hdibenzo[aj]xanthene derivatives by the reaction of 2-naphtol and aldehydes. Different types of aromatic and aliphatic aldehydes are used in the reaction and in all cases the products were obtained in good to excellent yields.展开更多
The modification of graphitic carbon nitride can significantly improve the photocatalytic performance of graphitic carbon nitride(g-C3N4).Fe2O3/nitrogen-deficient g-C3N4-x composite catalysts were prepared with dicyan...The modification of graphitic carbon nitride can significantly improve the photocatalytic performance of graphitic carbon nitride(g-C3N4).Fe2O3/nitrogen-deficient g-C3N4-x composite catalysts were prepared with dicyandiamide as the precursor and Fe3+doped in this study.The composite catalysts were characterized by XRD,SEM,FT-IR,XPS and photocurrent measurements.Close interaction occurred between Fe2O3 and nitrogen deficient g-C3N4-x,more photogenerated electrons were created and effectively separated from the holes,resulting in a decrease of photocarrier recombination,and thus enhancing the photocurrent.Photocatalytic performance experiments showed that Fe2O3/nitrogen deficient g-C3N4-x could utilize lowenergy visible light more efficiently than pure g-C3N4,and the removal rate was 92%in 60 minutes.展开更多
A bifunctional Co modified Fe3O4-Mn catalyst was prepared for Fischer-Tropsch synthesis (FTS). The influence of Co loading on the synergistic effect of Fe-Co as well as FTS performance over Fe1CoxMn1 catalysts was stu...A bifunctional Co modified Fe3O4-Mn catalyst was prepared for Fischer-Tropsch synthesis (FTS). The influence of Co loading on the synergistic effect of Fe-Co as well as FTS performance over Fe1CoxMn1 catalysts was studied. Incorporation of Co species into the Fe3O4-Mn catalyst promoted the reduction of iron oxides, increasing iron active sites during FTS. Moreover, the adding of Co species enhanced the electron transfer from Fe to Co metal, which strengthened the synergistic effect of Fe-Co, improving the catalytic performance. The Fe1CoxMn1 catalyst with higher Co loading promoted further the hydrogenation ability, favoring the shifting of the product distribution towards shorter hydrocarbons. Under optimized conditions of 280℃, 2.0 MPa and 3000 h-1, the highest yield of liquid fuels was obtained for the Fe1Co1Mn1 catalyst.展开更多
The Ni-Al2O3 catalyst was prepared by the mechanochemical method in combination with a planetary ballmilling machine.Effect of milling time on the crystal structure,the reduction characteristics and the catalytic perf...The Ni-Al2O3 catalyst was prepared by the mechanochemical method in combination with a planetary ballmilling machine.Effect of milling time on the crystal structure,the reduction characteristics and the catalytic performance of Ni-Al2O3 catalyst for hydrogenation of 1,4-butynediol to produce 1,4-butenediol were investigated.The catalysts were characterized by PSD,EDX,XRD,H2-TPR,BET,TEM,and NH3-TPD methods.Results showed that the MCt2.5 catalyst treated at a ball milling time of 2.5 h could form a smallest particle size of 191.0 nm.The evaluation experiments revealed that the activity of the prepared catalyst increased at first and then reached a constant value with the extension of ballmilling time.The BYD conversion,BED selectivity and yield on the MCt2.5 catalyst reached 35.63%,33.48%and 32.46%,respectively,which were higher than those obtained by other samples.The excellent performance of MCt2.5 sample is mainly related to the following three reasons from characterization results.Firstly,it has a smallest particle size of 191.0 nm;and then,the surface acidity(in terms of strong acids)of the catalyst was weaker than other catalysts;and eventually,the loading amount(23.84%)of the active component Ni exceeded the theoretical value(20%).展开更多
The magnetically separable ternary polyetherimide/titanate@Fe3O4(PTF) photocatalysts of special heterostructure between magnetite(Fe3O4) microspheres and titanates nanosheets modified by polyetherimide(PEI) were succe...The magnetically separable ternary polyetherimide/titanate@Fe3O4(PTF) photocatalysts of special heterostructure between magnetite(Fe3O4) microspheres and titanates nanosheets modified by polyetherimide(PEI) were successfully fabricated via a simple facile hydrothermal deposition method. The as-prepared photocatalysts were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, Transmission electron microscopy and UV-vis diffuse reflectance spectroscopy etc. The results showed that the as-fabricated material had a structure of Fe3O4microspheres coated with titanates nanosheets modified by PEI. The special interfacial contact between 3 D microsphere and 2 D nanosheets in the nanoarchitectures was formed via electrostatic attraction. Furthermore, the resulted photocatalysts were tested by degradation reaction of methylene blue under visible light irradiation and demonstrated an enhanced performance than the pure Fe3O4microspheres, and the photocatalytic activity enhanced with the molar ratio of Fe3O4microspheres and modified titanate gradually, which was attributed to the expansion of the surface area and the different electrostatic contact between the Fe3O4microspheres and titanate nanosheets. Moreover, the obtained results revealed the high yield magnetic separation and efficient reusability of PTF-5(96.7%) over 3 times reuse.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 (21203017)Open Fund of State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences (N-11-3)+1 种基金Program for Liaoning Excellent Talents in University (LNET)the Funda-mental Research Funds for the Central Universities (DC201502020304)~~
文摘separation is an attractive alternative to filtration or centrifugation for separating solid catalysts from a liquid phase, Here, core-shell Fe3O4@UiO-66-NH2 nanohybrids with well-defined structures were constructed by dispersing magnets in a dimethylformamide （DMF） solution con- taining two metal-organic framework （MOF） precursors, namely ZrCI4 and 2-aminobenzenetricar- boxylic acid. This method is simpler and more efficient than previously reported step-by-step method in which magnets were consecutively dispersed in DMF solutions each containing one MOF precursor, and the obtained Fe304@UiO-66-NH2 with three assembly cycles has a higher degree of crystallinity and porosiW. The core-shell Fe3O4@UiO-66-NH2 is highly active and selective in Knoevenagel condensations because of the bifunctionality of UiO-66-NH2 and better mass transfer in the nano-sized shells. It also has good recycling stability, and can be recovered magnetically and reused at least four times without significant loss of catalytic activity and framework integrity. The effects of substitution on the reactivity of benzaldehyde and of substrate size were also investigated.
基金supported by the National Natural Science Foundation of China (Nos. 50872011, 50402022, and 50672006)the National Basic Research Program of China (No. 2007CB613608)
文摘Nano TiO2/Fe3O4 composite particles with different molar ratios of TiO2 to Fe3O4 were prepared via sol-gel method. X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry were used to characterize the TiO2/Fe3O4 particles. The photocatalytic activity of the particles was tested by degrading methyl blue solution under UV illumination （254 nm）. The results indicate that with the content of TiO2 increasing, the photocatalytic activity of the composite particles enhances, while the magnetism of the particles decreases. When the molar ratio of TiO2 to Fe3O4 is about 8, both the photocatalytic activity and magnetism of the TiO2/Fe3O4 particles are relatively high, and their photocatalytic activity remains well after repeated use.
文摘Several catalysts comprising Pt supported on octahedral Fe3O4（Pt/Fe3O4） were prepared by a facile method involving co-precipitation followed by thermal treatment at different temperatures. A variety of characterization results revealed that this preparation process afforded highly crystalline octahedral Fe3O4 with a uniform distribution of Pt nanoparticles on its surface. The thermal-treatment temperature significantly influenced the redox properties of the Pt/Fe3O4 catalysts. All the Pt/Fe3O4 catalysts were found to be catalytically active and stable for the oxidation of low-concentration formaldehyde（HCHO） with oxygen. The catalyst prepared by thermal treatment at 80 °C（labelled Pt/Fe3O4-80） exhibited the highest catalytic activity, efficiently converting HCHO to CO2 and H2 O under ambient temperature and moisture conditions. The excellent performance of Pt/Fe3O4-80 was mainly attributed to beneficial interactions between the Pt and Fe species that result in the formation a higher density of active interface sites（e.g., Pt-O-FeO x and Pt-OH-FeO x）. The introduction of water vapor improves the catalytic activity of the Pt/Fe3O4 catalysts as it participates in a water-assisted dissociation process.
文摘Biodiesel is a green fuel which can replace diesel while addressing various issues such as scarcity of hydrocarbon fuels and environmental pollution to an extent. The high production cost of biodiesel and the recovery of the catalyst after the transesterification process are the major challenges to be addressed in biodiesel production. In the present work, a cheap and promising solid base oxide catalyst was synthesized from chicken eggshell by calcination at 900 ℃ forming catalyst eggshells(CES) and was impregnated with the nanomagnetic material(Fe3O4) to obtain Fe3O4 loaded catalytic eggshell(CES–Fe3O4). Fe3O4 nanomaterials were synthesized by co-precipitation method and were loaded in catalytic eggshell by sonication, for better recovery of the catalyst after transesterification process. CES–Fe3O4 material was characterized by Thermogravimetric analysis, X-ray diffraction, Fourier transform infrared spectroscopy, a vibrating-sample magnetometer, Brunauer-Emmett-Teller, Dynamic light scattering, and Scanning electron microscopy. Biodiesel was synthesized by transesterification of Pongamia pinnata raw oil with 1:12 oil to methanol molar ratio and 2 wt% catalyst loading for 2 h at a temperature of 65 ℃ and yields were compared. The reusability of the catalyst was studied by the transesterification of the raw oil and its catalytic activity was found to be retained up to 7 cycles with a yield of 98%.
文摘Fe（HSO4）3 has been used as an efficient and recyclable catalyst for the one-pot synthesis of 14-aryl- or alkyl-14Hdibenzo[aj]xanthene derivatives by the reaction of 2-naphtol and aldehydes. Different types of aromatic and aliphatic aldehydes are used in the reaction and in all cases the products were obtained in good to excellent yields.
基金Supported by the Fuling Shale Gas Environmental Exploration Technology of National Science and Technology Special Project(No.2016ZX05060)the Demonstration of Integrated Management of Rocky Desertification and Enhancement of Ecological Service Function in Karst Peak-cluster Depression(No.2016YFC0502400)National Natural Science Foundation of China(No.51709254)
文摘The modification of graphitic carbon nitride can significantly improve the photocatalytic performance of graphitic carbon nitride(g-C3N4).Fe2O3/nitrogen-deficient g-C3N4-x composite catalysts were prepared with dicyandiamide as the precursor and Fe3+doped in this study.The composite catalysts were characterized by XRD,SEM,FT-IR,XPS and photocurrent measurements.Close interaction occurred between Fe2O3 and nitrogen deficient g-C3N4-x,more photogenerated electrons were created and effectively separated from the holes,resulting in a decrease of photocarrier recombination,and thus enhancing the photocurrent.Photocatalytic performance experiments showed that Fe2O3/nitrogen deficient g-C3N4-x could utilize lowenergy visible light more efficiently than pure g-C3N4,and the removal rate was 92%in 60 minutes.
基金supported by International Cooperation and Exchange Program of the National Natural Science Foundation of China(No.51861145102)Science and Technology Program of Shenzhen(No.JCYJ20180302153928437)Fundamental Research Fund for the Central Universities(No.2042019kf0221)
文摘A bifunctional Co modified Fe3O4-Mn catalyst was prepared for Fischer-Tropsch synthesis (FTS). The influence of Co loading on the synergistic effect of Fe-Co as well as FTS performance over Fe1CoxMn1 catalysts was studied. Incorporation of Co species into the Fe3O4-Mn catalyst promoted the reduction of iron oxides, increasing iron active sites during FTS. Moreover, the adding of Co species enhanced the electron transfer from Fe to Co metal, which strengthened the synergistic effect of Fe-Co, improving the catalytic performance. The Fe1CoxMn1 catalyst with higher Co loading promoted further the hydrogenation ability, favoring the shifting of the product distribution towards shorter hydrocarbons. Under optimized conditions of 280℃, 2.0 MPa and 3000 h-1, the highest yield of liquid fuels was obtained for the Fe1Co1Mn1 catalyst.
基金This work has been supported by the Xinjiang Uygur Autonomous Region Key R&D Program(2017B02012)the Xinjiang University Natural Science Foundation Project(BS160221).
文摘The Ni-Al2O3 catalyst was prepared by the mechanochemical method in combination with a planetary ballmilling machine.Effect of milling time on the crystal structure,the reduction characteristics and the catalytic performance of Ni-Al2O3 catalyst for hydrogenation of 1,4-butynediol to produce 1,4-butenediol were investigated.The catalysts were characterized by PSD,EDX,XRD,H2-TPR,BET,TEM,and NH3-TPD methods.Results showed that the MCt2.5 catalyst treated at a ball milling time of 2.5 h could form a smallest particle size of 191.0 nm.The evaluation experiments revealed that the activity of the prepared catalyst increased at first and then reached a constant value with the extension of ballmilling time.The BYD conversion,BED selectivity and yield on the MCt2.5 catalyst reached 35.63%,33.48%and 32.46%,respectively,which were higher than those obtained by other samples.The excellent performance of MCt2.5 sample is mainly related to the following three reasons from characterization results.Firstly,it has a smallest particle size of 191.0 nm;and then,the surface acidity(in terms of strong acids)of the catalyst was weaker than other catalysts;and eventually,the loading amount(23.84%)of the active component Ni exceeded the theoretical value(20%).
基金Funded by the National Natural Science Foundation of China(Nos.21103054,21003055,and 50872037)the Open Fund of Fujian Provincial Key Laboratory of Functional Materials and Applications(Xiamen University of Technology)(No.608160030215)the Program for Innovative Research Team in Science and Technology in Fujian Province University(IRTSTFJ)
文摘The magnetically separable ternary polyetherimide/titanate@Fe3O4(PTF) photocatalysts of special heterostructure between magnetite(Fe3O4) microspheres and titanates nanosheets modified by polyetherimide(PEI) were successfully fabricated via a simple facile hydrothermal deposition method. The as-prepared photocatalysts were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, Transmission electron microscopy and UV-vis diffuse reflectance spectroscopy etc. The results showed that the as-fabricated material had a structure of Fe3O4microspheres coated with titanates nanosheets modified by PEI. The special interfacial contact between 3 D microsphere and 2 D nanosheets in the nanoarchitectures was formed via electrostatic attraction. Furthermore, the resulted photocatalysts were tested by degradation reaction of methylene blue under visible light irradiation and demonstrated an enhanced performance than the pure Fe3O4microspheres, and the photocatalytic activity enhanced with the molar ratio of Fe3O4microspheres and modified titanate gradually, which was attributed to the expansion of the surface area and the different electrostatic contact between the Fe3O4microspheres and titanate nanosheets. Moreover, the obtained results revealed the high yield magnetic separation and efficient reusability of PTF-5(96.7%) over 3 times reuse.
