Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, ...Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, N2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pt nanoparticles were highly dispersed in the CMK-3 with 43.7% dispersion. The Pt/CMK-3 catalyst was an effective catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives under the experimental conditions studied here. The Pt/CMK-3 catalyst was more active than commercial Pt/C catalyst in most cases. A highest turnover frequency of 43.8 s-1 was measured when the Pt/CMK-3 catalyst was applied for the hydrogenation of 2-methyl-nitrobenzene in ethanol under optimal conditions. It is worthy of note that the Pt/CMK-3 catalyst could be recycled easily, and could be reused at least fourteen times without any loss in activity or selectivity for the hydrogenation of nitrobenzene in ethanol.展开更多
Ni supported on bentonite was prepared by the impregnation method with different nickel contents, applied to the hydrogenation of nitrobenzene to aniline in a fixed-bed reactor, and it was characterized by X-ray diffr...Ni supported on bentonite was prepared by the impregnation method with different nickel contents, applied to the hydrogenation of nitrobenzene to aniline in a fixed-bed reactor, and it was characterized by X-ray diffraction(XRD), H2-temperature programmed reduction(H2-TPR), and X-ray photoelectron spectrometry(XPS). The results showed that Ni/bentonite catalyst with 20 wt% nickel content provided a higher conversion of nitrobenzene and selectivity of aniline compared to other catalysts. NiO was the precursor of the active component of the catalyst, and the small crystallite size as well as the highly dispersed NiO on the Ni/bentonite-20 catalyst, contributed to the catalytic performance. The hydrogenation of nitrobenzene was carried out at 300℃ with a H_2 gaseous hourly space velocity of 4800 ml·(g cat)^-1·h^-1and a nitrobenzene liquid hourly space velocity of4.8 ml·(g cat)^-1·h^-1 over Ni/bentonite-20. A 95.7% nitrobenzene conversion and 98.8% aniline selectivity were obtained. While the nitrobenzene liquid hourly space velocity was 4.8 ml·(g cat)^-1·h^-1, the yield of aniline was more than 95.0% during a 10-hour reaction.展开更多
The Ag/γ-Fe_2O_3 nanocomposite was synthesized by solvothermal reduction method via using ferric nitrate and silver nitrate as raw materials, and ethylene glycol as the reducing agent. The composite was characterized...The Ag/γ-Fe_2O_3 nanocomposite was synthesized by solvothermal reduction method via using ferric nitrate and silver nitrate as raw materials, and ethylene glycol as the reducing agent. The composite was characterized by X-ray powder diffraction, scanning electron microscope, transmission electron microscope, and energy dispersive X-ray. The prepared Ag/γ-Fe_2O_3 was used for the catalytic hydrogenation of nitrobenzene to aniline by hydrazine hydrate. The factors such as the silver content in the catalyst, reaction time, reaction temperature and the regeneration of catalyst were investigated. The results showed that the yield of aniline reached 100% by utilizing the 1%wt(nitrobenzene) Ag/γ-Fe_2O_3 for the catalytic hydrogenation of nitrobenzene for 3 h to obtain aniline at 78 ℃, hydrazine hydrate as the hydrogen source, while the silver content in the catalyst was 3%mol.展开更多
The Shanxi Institute of Coal Chemistry,Chinese Academy of Sciences has designed and prepared a multiple confined-zone-based nickel hydrogenation catalyst by means of the atomic layer deposition(ALD)technology.In compa...The Shanxi Institute of Coal Chemistry,Chinese Academy of Sciences has designed and prepared a multiple confined-zone-based nickel hydrogenation catalyst by means of the atomic layer deposition(ALD)technology.In comparison with the non-confined-zone based catalyst,the multiple confined-zone-based nickel catalyst possesses an enhanced catalytic reactivity and catalytic stability for hydrogenation of cinnamaldehyde and nitrobenzene.展开更多
This study used nitrobenzene as the simulated pollutant to study the effects of common inorganic sodium salts and organics on nitrobenzene degradation by O_3/H_2O_2 in high-gravity fields. The experiment results showe...This study used nitrobenzene as the simulated pollutant to study the effects of common inorganic sodium salts and organics on nitrobenzene degradation by O_3/H_2O_2 in high-gravity fields. The experiment results showed that the highgravity technology could increase the nitrobenzene removal rate by improving the ozone transfer efficiency and ozone dissolution. Coexisting substances had different effects on the degradation kinetics of nitrobenzene in high-gravity fields. Among such substances, Na_2CO_3, NaOH, Na_3PO_4, and NaNO_3 accelerated the removal of nitrobenzene. The main action principle of nitrobenzene degradation by O_3/H_2O_2 is that the additives can increase the pH value of the solution, stimulate ozonolysis, generate hydroxyl radicals(·OH), and improve oxidation efficiency. By contrast, NaCl, NaHCO_3, NaHSO_4, ethanol(C_2H_5OH), acetic acid(CH_3COOH), formic acid(HCOOH), and tert-butyl alcohol(TBA) inhibited nitrobenzene removal. When NaHCO_3, CH_3COOH, or HCOOH were added, the pH value of the solution decreased and free radical chain reactions were hindered. However, NaCl, NaHCO_3, C_2H_5OH, and TBA consumed ·OH radicals and inhibited nitrobenzene removal.展开更多
A series of Cu-doped La-Ni intermetallic compounds(LaN5-xCux, x = 0-4) was studied. The bulk structure and surface composition of the samples were detected before and after they were used as catalyst for nitrobenzene ...A series of Cu-doped La-Ni intermetallic compounds(LaN5-xCux, x = 0-4) was studied. The bulk structure and surface composition of the samples were detected before and after they were used as catalyst for nitrobenzene hydrogennation. The catalytic properties of the intermetallic compounds depend on the surface region composition, especially on the valence of the metal ions.展开更多
The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supp...The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.展开更多
基金supported by the National Natural Science Foundation of China(21273076 and 21373089)the Open Research Fund of Top Key Discipline of Chemistry in Zhejiang Provincial Colleges and Key Laboratory of the Ministry of Education for Catalysis Materials(Zhejiang Normal University,ZJHX2013)Shanghai Leading Academic Discipline Project (B409)~~
文摘Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, N2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pt nanoparticles were highly dispersed in the CMK-3 with 43.7% dispersion. The Pt/CMK-3 catalyst was an effective catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives under the experimental conditions studied here. The Pt/CMK-3 catalyst was more active than commercial Pt/C catalyst in most cases. A highest turnover frequency of 43.8 s-1 was measured when the Pt/CMK-3 catalyst was applied for the hydrogenation of 2-methyl-nitrobenzene in ethanol under optimal conditions. It is worthy of note that the Pt/CMK-3 catalyst could be recycled easily, and could be reused at least fourteen times without any loss in activity or selectivity for the hydrogenation of nitrobenzene in ethanol.
基金Supported by the National Natural Science Foundation of China(21566005,21425627)Natural Science Foundation of Guangxi province(2014GXNSFAA118049)+1 种基金the Open Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2013K011)the Patent Project of Colleges and Universities of Guangxi Zhuang Autonomous Region(KY2015ZL001)
文摘Ni supported on bentonite was prepared by the impregnation method with different nickel contents, applied to the hydrogenation of nitrobenzene to aniline in a fixed-bed reactor, and it was characterized by X-ray diffraction(XRD), H2-temperature programmed reduction(H2-TPR), and X-ray photoelectron spectrometry(XPS). The results showed that Ni/bentonite catalyst with 20 wt% nickel content provided a higher conversion of nitrobenzene and selectivity of aniline compared to other catalysts. NiO was the precursor of the active component of the catalyst, and the small crystallite size as well as the highly dispersed NiO on the Ni/bentonite-20 catalyst, contributed to the catalytic performance. The hydrogenation of nitrobenzene was carried out at 300℃ with a H_2 gaseous hourly space velocity of 4800 ml·(g cat)^-1·h^-1and a nitrobenzene liquid hourly space velocity of4.8 ml·(g cat)^-1·h^-1 over Ni/bentonite-20. A 95.7% nitrobenzene conversion and 98.8% aniline selectivity were obtained. While the nitrobenzene liquid hourly space velocity was 4.8 ml·(g cat)^-1·h^-1, the yield of aniline was more than 95.0% during a 10-hour reaction.
基金supported by the science and technology support project of Jiangsu Province(No.BY2015057-03)
文摘The Ag/γ-Fe_2O_3 nanocomposite was synthesized by solvothermal reduction method via using ferric nitrate and silver nitrate as raw materials, and ethylene glycol as the reducing agent. The composite was characterized by X-ray powder diffraction, scanning electron microscope, transmission electron microscope, and energy dispersive X-ray. The prepared Ag/γ-Fe_2O_3 was used for the catalytic hydrogenation of nitrobenzene to aniline by hydrazine hydrate. The factors such as the silver content in the catalyst, reaction time, reaction temperature and the regeneration of catalyst were investigated. The results showed that the yield of aniline reached 100% by utilizing the 1%wt(nitrobenzene) Ag/γ-Fe_2O_3 for the catalytic hydrogenation of nitrobenzene for 3 h to obtain aniline at 78 ℃, hydrazine hydrate as the hydrogen source, while the silver content in the catalyst was 3%mol.
文摘The Shanxi Institute of Coal Chemistry,Chinese Academy of Sciences has designed and prepared a multiple confined-zone-based nickel hydrogenation catalyst by means of the atomic layer deposition(ALD)technology.In comparison with the non-confined-zone based catalyst,the multiple confined-zone-based nickel catalyst possesses an enhanced catalytic reactivity and catalytic stability for hydrogenation of cinnamaldehyde and nitrobenzene.
基金supported by the Natural Science Foundation of China(21206153,U1610106)the Excellent Youth Science and Technology Foundation of Province Shanxi of China(2014021007)the Program for the Outstanding Innovative Teams of Higher Learning Institutions of Shanxi(201316)
文摘This study used nitrobenzene as the simulated pollutant to study the effects of common inorganic sodium salts and organics on nitrobenzene degradation by O_3/H_2O_2 in high-gravity fields. The experiment results showed that the highgravity technology could increase the nitrobenzene removal rate by improving the ozone transfer efficiency and ozone dissolution. Coexisting substances had different effects on the degradation kinetics of nitrobenzene in high-gravity fields. Among such substances, Na_2CO_3, NaOH, Na_3PO_4, and NaNO_3 accelerated the removal of nitrobenzene. The main action principle of nitrobenzene degradation by O_3/H_2O_2 is that the additives can increase the pH value of the solution, stimulate ozonolysis, generate hydroxyl radicals(·OH), and improve oxidation efficiency. By contrast, NaCl, NaHCO_3, NaHSO_4, ethanol(C_2H_5OH), acetic acid(CH_3COOH), formic acid(HCOOH), and tert-butyl alcohol(TBA) inhibited nitrobenzene removal. When NaHCO_3, CH_3COOH, or HCOOH were added, the pH value of the solution decreased and free radical chain reactions were hindered. However, NaCl, NaHCO_3, C_2H_5OH, and TBA consumed ·OH radicals and inhibited nitrobenzene removal.
文摘A series of Cu-doped La-Ni intermetallic compounds(LaN5-xCux, x = 0-4) was studied. The bulk structure and surface composition of the samples were detected before and after they were used as catalyst for nitrobenzene hydrogennation. The catalytic properties of the intermetallic compounds depend on the surface region composition, especially on the valence of the metal ions.
基金the National Key R&D Program of China(2018YFA0702003)the National Natural Science Foundation of China(21890383,21671117,21871159 and21901135)the Science and Technology Key Project of Guangdong Province of China(2020B010188002)。
文摘The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.