In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can r...In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.展开更多
Silane coupling agent KH560 was used to modify the surface of nano-α-Al<sub>2</sub>O<sub>3</sub> in ethanol-aqueous solution with different proportions. The particle size of nano-α-Al<sub&...Silane coupling agent KH560 was used to modify the surface of nano-α-Al<sub>2</sub>O<sub>3</sub> in ethanol-aqueous solution with different proportions. The particle size of nano-α-Al<sub>2</sub>O<sub>3</sub> was determined by nano-particle size analyzer, and the effects of nano-α-Al<sub>2</sub>O<sub>3</sub> content, ethanol-aqueous solution ratio and KH560 dosage on the dispersion and particle size of nano-α-Al<sub>2</sub>O<sub>3</sub> were investigated. The material structure before and after modification was determined by Fourier transform infrared spectroscopy (FTIR). Aqueous polyurethane resin and inorganic components are combined with modified nano-α-Al<sub>2</sub>O<sub>3</sub> dispersion to form chromium-free passivation solution. The solution is coated on the galvanized sheet, the adhesion and surface hardness are tested, the bonding strength of the coating and the surface hardness of the substrate are discussed. The corrosion resistance and surface morphology of the matrix were investigated by electrochemical test, neutral salt spray test and scanning electron microscope test. The chromium-free passivation film formed after the modification of nano-α-Al<sub>2</sub>O<sub>3</sub> increases the surface hardness of galvanized sheet by about 85%. The corrosion resistance of the film is better than that of a single polyurethane film. The results show that the surface hardness and corrosion resistance of polyurethane resin composite passivation film are significantly improved by the introduction of nano-α-Al<sub>2</sub>O<sub>3</sub>.展开更多
Ag3PO4/Ag/Ag2Mo2O7 composite photocatalyst was successfully prepared via an in situ precipitation method. The as-prepared Ag3PO4/Ag/Ag2Mo2O7 nanocomposite included Ag3PO4 nanoparticles (NPs) as well as Ag NPs assemb...Ag3PO4/Ag/Ag2Mo2O7 composite photocatalyst was successfully prepared via an in situ precipitation method. The as-prepared Ag3PO4/Ag/Ag2Mo2O7 nanocomposite included Ag3PO4 nanoparticles (NPs) as well as Ag NPs assembling on the surface of Ag2Mo2O7 nanowires. Under visible light irradiation (λ〉420 nm), the Ag3PO4/Ag/Ag2Mo2O7 com- posite degraded rhodamine B (Rh B) efficiently and showed much higher photocatalytic efficiency than pure AgaPO4, Ag2Mo2O7, or Ag3PO4/Ag2Mo2O7. It was elucidated that the excellent photocatalytic performance of Ag3PO4/Ag/Ag2Mo2O7 for the degradation of Rh B under visible light could be ascribed to the high specific surface area, the extended absorption in the visible light region resulting from the Ag3PO4/Ag loading, and the effi- cient separation of photogenerated electrons and holes through the ternary heterostrucure composed of Ag3PO4, Ag and Ag2Mo2O7.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
In this investigation, Pt–Ba–Ce/c-Al2O3 catalysts were prepared by incipient wetness impregnation and experiments were performed to evaluate the influence of H2 on the evolution mechanism of nitrogen oxides (NOx) st...In this investigation, Pt–Ba–Ce/c-Al2O3 catalysts were prepared by incipient wetness impregnation and experiments were performed to evaluate the influence of H2 on the evolution mechanism of nitrogen oxides (NOx) storage and reduction (NSR). The physical and chemical properties of the Pt–Ba–Ce/c- Al2O3 catalysts were studied using a combination of characterization techniques, which showed that PtOx, CeO2, and BaCO3, whose peaks were observed in X-ray diffraction (XRD) spectra, dispersed well on the c-Al2O3, as shown by transmission electron microscope (TEM), and that the difference between Ce3+ and Ce4+, as detected by X-ray photoelectron spectroscopy (XPS), facilitated the migration of active oxygen over the catalyst. In the process of a complete NSR experiment, the NOx storage capability was greatly enhanced in the temperature range of 250–350℃, and reached a maximum value of 315.3μmol·gcat^-1 at 350℃, which was ascribed to the increase in NO2 yield. In a lean and rich cycling experiment, the results showed that NOx storage efficiency and conversion were increased when the time of H2 exposure (i.e., 30, 45, and 60 s) was extended. The maximum NOx conversion of the catalyst reached 83.5% when the duration of the lean and rich phases was 240 and 60 s, respectively. The results revealed that increasing the content of H2 by an appropriate amount was favorable to the NSR mechanism due to increased decomposition of nitrate or nitrite, and the refreshing of trapping sites for the next cycle of NSR.展开更多
Mesoporous Pb3Nb2O8 photocatalysts were synthesized by the evaporation‐induced self‐assembly (EISA) method. Ag was deposited on the surface of mesoporous Pb3Nb2O8 by a facile photoreduction process. The as‐prepared...Mesoporous Pb3Nb2O8 photocatalysts were synthesized by the evaporation‐induced self‐assembly (EISA) method. Ag was deposited on the surface of mesoporous Pb3Nb2O8 by a facile photoreduction process. The as‐prepared samples were characterized by TG‐DSC, XRD, N2 adsorption, HR‐TEM andUV‐Vis spectroscopy. The results revealed that mesoporous Pb3Nb2O8 has a large specific surfacearea and uniform pore size distribution both before and after Ag deposition. The photodegradationof 2‐propanol and acetaldehyde gas under visible‐light (λ > 420 nm) irradiation was employed toevaluate the photocatalytic activities of the samples. The results showed that the photocatalyticactivity of mesoporous Pb3Nb2O8 is greatly improved by the Ag co‐catalyst. These mesoporousPb3Nb2O8 exhibit photocatalytic activities as much as 41 times higher when compared with thePb3Nb2O8 prepared by the solid state reaction method. The content of loaded Ag ranged from 0.5%to 5% (Ag2SO4). The optimal loading was determined to be 1% corresponding the highest photocatalyti cactivity. These results clearly indicate that the activity of Pb3Nb2O8 can be improved to obtain an outstanding performance for the photodegradation of organic pollutants.展开更多
An efficient route for the synthesis of 5-substituted 1H-tetrazole via[2+3]cycloaddition of nitriles and sodium azide is reported usingγ-Fe2O3 nanoparticles as a magnetic separable catalyst.Under optimized condition...An efficient route for the synthesis of 5-substituted 1H-tetrazole via[2+3]cycloaddition of nitriles and sodium azide is reported usingγ-Fe2O3 nanoparticles as a magnetic separable catalyst.Under optimized conditions,the moderate to good yields(71-95%) can be obtained.The catalyst can be easily separated by a magnet and reused for several circles.展开更多
基金financial support from National Natural Science Foundation of China(Nos.52004102 and 22078125)Postdoctoral Science Foundation of China(No.2021M690068)+2 种基金Fundamental Research Funds for the Central Universities(Nos.JUSRP221018 and JUSRP622038)Key Laboratory of Green Cleaning Technology and Detergent of Zhejiang Province(No.Q202204)Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(No.GCP202112)。
文摘In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.
文摘Silane coupling agent KH560 was used to modify the surface of nano-α-Al<sub>2</sub>O<sub>3</sub> in ethanol-aqueous solution with different proportions. The particle size of nano-α-Al<sub>2</sub>O<sub>3</sub> was determined by nano-particle size analyzer, and the effects of nano-α-Al<sub>2</sub>O<sub>3</sub> content, ethanol-aqueous solution ratio and KH560 dosage on the dispersion and particle size of nano-α-Al<sub>2</sub>O<sub>3</sub> were investigated. The material structure before and after modification was determined by Fourier transform infrared spectroscopy (FTIR). Aqueous polyurethane resin and inorganic components are combined with modified nano-α-Al<sub>2</sub>O<sub>3</sub> dispersion to form chromium-free passivation solution. The solution is coated on the galvanized sheet, the adhesion and surface hardness are tested, the bonding strength of the coating and the surface hardness of the substrate are discussed. The corrosion resistance and surface morphology of the matrix were investigated by electrochemical test, neutral salt spray test and scanning electron microscope test. The chromium-free passivation film formed after the modification of nano-α-Al<sub>2</sub>O<sub>3</sub> increases the surface hardness of galvanized sheet by about 85%. The corrosion resistance of the film is better than that of a single polyurethane film. The results show that the surface hardness and corrosion resistance of polyurethane resin composite passivation film are significantly improved by the introduction of nano-α-Al<sub>2</sub>O<sub>3</sub>.
基金supported by the National Natural Science Foundation of China(No.21407059,No.21576112,No.21407064,and No.21607051)the Science Development Project of Jiangsu Province(BK20140527)+1 种基金the Science and Technology Research Project of the Department of Education of Jilin Province(No.2015220)the Open Subject of the State Key Laboratory of Rare Earth Resource Utilization(RERU2017011)
文摘Ag3PO4/Ag/Ag2Mo2O7 composite photocatalyst was successfully prepared via an in situ precipitation method. The as-prepared Ag3PO4/Ag/Ag2Mo2O7 nanocomposite included Ag3PO4 nanoparticles (NPs) as well as Ag NPs assembling on the surface of Ag2Mo2O7 nanowires. Under visible light irradiation (λ〉420 nm), the Ag3PO4/Ag/Ag2Mo2O7 com- posite degraded rhodamine B (Rh B) efficiently and showed much higher photocatalytic efficiency than pure AgaPO4, Ag2Mo2O7, or Ag3PO4/Ag2Mo2O7. It was elucidated that the excellent photocatalytic performance of Ag3PO4/Ag/Ag2Mo2O7 for the degradation of Rh B under visible light could be ascribed to the high specific surface area, the extended absorption in the visible light region resulting from the Ag3PO4/Ag loading, and the effi- cient separation of photogenerated electrons and holes through the ternary heterostrucure composed of Ag3PO4, Ag and Ag2Mo2O7.
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the National Natural Science Foundation of China (51676090)the Natural Science Foundation of Jiangsu Province (BK20150513), and the Six Talent Peaks Project in Jiangsu Province.
文摘In this investigation, Pt–Ba–Ce/c-Al2O3 catalysts were prepared by incipient wetness impregnation and experiments were performed to evaluate the influence of H2 on the evolution mechanism of nitrogen oxides (NOx) storage and reduction (NSR). The physical and chemical properties of the Pt–Ba–Ce/c- Al2O3 catalysts were studied using a combination of characterization techniques, which showed that PtOx, CeO2, and BaCO3, whose peaks were observed in X-ray diffraction (XRD) spectra, dispersed well on the c-Al2O3, as shown by transmission electron microscope (TEM), and that the difference between Ce3+ and Ce4+, as detected by X-ray photoelectron spectroscopy (XPS), facilitated the migration of active oxygen over the catalyst. In the process of a complete NSR experiment, the NOx storage capability was greatly enhanced in the temperature range of 250–350℃, and reached a maximum value of 315.3μmol·gcat^-1 at 350℃, which was ascribed to the increase in NO2 yield. In a lean and rich cycling experiment, the results showed that NOx storage efficiency and conversion were increased when the time of H2 exposure (i.e., 30, 45, and 60 s) was extended. The maximum NOx conversion of the catalyst reached 83.5% when the duration of the lean and rich phases was 240 and 60 s, respectively. The results revealed that increasing the content of H2 by an appropriate amount was favorable to the NSR mechanism due to increased decomposition of nitrate or nitrite, and the refreshing of trapping sites for the next cycle of NSR.
基金supported by the National Natural Science Foundation of China (11274150, 11574124)the Education Minister of Liaoning Province (JG2016ZD0015)the Open Research Fund of Jiangsu Provincial Key Laboratory for Nanotechnology Nanjing University~~
文摘Mesoporous Pb3Nb2O8 photocatalysts were synthesized by the evaporation‐induced self‐assembly (EISA) method. Ag was deposited on the surface of mesoporous Pb3Nb2O8 by a facile photoreduction process. The as‐prepared samples were characterized by TG‐DSC, XRD, N2 adsorption, HR‐TEM andUV‐Vis spectroscopy. The results revealed that mesoporous Pb3Nb2O8 has a large specific surfacearea and uniform pore size distribution both before and after Ag deposition. The photodegradationof 2‐propanol and acetaldehyde gas under visible‐light (λ > 420 nm) irradiation was employed toevaluate the photocatalytic activities of the samples. The results showed that the photocatalyticactivity of mesoporous Pb3Nb2O8 is greatly improved by the Ag co‐catalyst. These mesoporousPb3Nb2O8 exhibit photocatalytic activities as much as 41 times higher when compared with thePb3Nb2O8 prepared by the solid state reaction method. The content of loaded Ag ranged from 0.5%to 5% (Ag2SO4). The optimal loading was determined to be 1% corresponding the highest photocatalyti cactivity. These results clearly indicate that the activity of Pb3Nb2O8 can be improved to obtain an outstanding performance for the photodegradation of organic pollutants.
基金the Jiangsu Province Foundation of Natural Science(No.BK2009678) for the financial support
文摘An efficient route for the synthesis of 5-substituted 1H-tetrazole via[2+3]cycloaddition of nitriles and sodium azide is reported usingγ-Fe2O3 nanoparticles as a magnetic separable catalyst.Under optimized conditions,the moderate to good yields(71-95%) can be obtained.The catalyst can be easily separated by a magnet and reused for several circles.