A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactiva...A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactivation of the catalysts were studied. N2 adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, H2 temperature‐programmed reduction, NH3 temperature‐programmed desorption, X‐ray photoelectron spectroscopy (XPS), thermal gravimetric analysis and Fourier transform infrared spectroscopy were used to character‐ize the catalysts. The 8Fe‐8Mn/Al2O3 catalyst gave 99%of NO conversion at 150?? and more than 92.6%NO conversion was obtained in a wide low temperature range of 90–210??. XPS analysis demonstrated that the Fe3+was the main iron valence state on the catalyst surface and the addition of Mn increased the accumulation of Fe on the surface. The higher specific surface area, enhanced dispersion of amorphous Fe and Mn, improved reduction properties and surface acidity, lower binding energy, higher Mn4+/Mn3+ratio and more adsorbed oxygen species resulted in higher NO conversion for the 8Fe‐8Mn/Al2O3 catalyst. In addition, the SCR activity of the 8Fe‐8Mn/Al2O3 cata‐lyst was only slightly decreased in the presence of H2O and SO2, which indicated that the catalyst had better tolerance to H2O and SO2. The reaction temperature was crucial for the SO2 resistance of catalyst and the decrease of catalytic activity caused by SO2 was mainly due to the sulfate salts formed on the catalyst.展开更多
Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high ca...Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high catalyst loadings required. In the present work, mesoporous Fe/N/C was syn- thesized through heat treatment of K]600 carbon black coated with poly-2-aminobenzimidazole and FeC13. The as-prepared Fe/N/C possesses a unique hollow-shell structure that contains a buffer zone allowing both water formation and vaporization, and also facilitates the mass transfer of gas- eous oxygen. This catalyst generated an oxygen reduction reaction activiW of 9.21 A/g in conjunc- tion with a peak power density of 0.71 W/cm2.展开更多
N2O is a promising green propellant and exhibits great potential for satellite propulsion systems. It is difficult for catalytic decomposition, which is an important way to initiate the propulsion process, to occur at...N2O is a promising green propellant and exhibits great potential for satellite propulsion systems. It is difficult for catalytic decomposition, which is an important way to initiate the propulsion process, to occur at temperatures below 600 °C due to the high activation energy of N2O. In this work, we report an Ir supported on rutile TiO2(Ir/r-TiO2) catalyst which exhibits a fairly high activity for high-concentration N2O decomposition. HAADF-STEM, H2-TPR, and XPS results indicate that highly dispersed Ir particles and improved oxygen mobility on the Ir/r-TiO2 could facilitate the decompo-sition of N2O and desorption of the adsorbed oxygen. Bridge-bonded peroxide intermediates were observed with in-situ DRIFT and herein, a detailed decomposition route is proposed.展开更多
Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with ...Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade.Despite substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied.Herein,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity.Finally,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are provided.In particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.展开更多
Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate ...Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate photocatalysts.Herein,a novel S-scheme Sb2WO6/g-C3N4 nanocomposite was fabricated by an ultrasound-assisted method,which exhibited excellent performance for photocatalytic ppb-level NO removal.Compared with the pure constituents of the nanocomposite,the as-prepared 15%-Sb2WO6/g-C3N4 photocatalyst could remove more than 68%continuous-flowing NO(initial concentration:400 ppb)under visible-light irradiation in 30 min.The findings of the trapping experiments confirmed that•O2^–and h+were the important active species in the NO oxidation reaction.Meanwhile,the transient photocurrent response and PL spectroscopy analyses proved that the unique S-scheme structure of the samples could enhance the charge separation efficiency.In situ DRIFTS revealed that the photocatalytic reaction pathway of NO removal over the Sb2WO6/g-C3N4 nanocomposite occurred via an oxygen-induced route.The present work proposes a new concept for fabricating efficient photocatalysts for photocatalytic ppb-level NO oxidation and provides deeper insights into the mechanism of photocatalytic NO oxidation.展开更多
A heterojunction photocatalyst based on porous tubular g-C3N4 decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method.The one-dimensional porous structure of g-C3N4 provides a hig...A heterojunction photocatalyst based on porous tubular g-C3N4 decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method.The one-dimensional porous structure of g-C3N4 provides a higher specific surface area,enhanced light absorption,and better separation and transport performance of charge carriers along the longitudinal direction,all of which synergistically contribute to the superior photocatalytic activity observed.The significantly enhanced catalytic efficiency is also a benefit originating from the fast transfer of photogenerated electrons and holes between g-C3N4 and CdS through a built-in electric field,which was confirmed by investigating the morphology,structure,optical properties,electrochemical properties,and photocatalytic activities.Photocatalytic degradation of rhodamine B(RhB)and photocatalytic hydrogen evolution reaction were also carried out to investigate its photocatalytic performance.RhB can be degraded completely within 60 min,and the optimum H2 evolution rate of tubular g-C3N4/CdS composite is as high as 71.6μmol h^–1,which is about 16.3 times higher than that of pure bulk g-C3N4.The as-prepared nanostructure would be suitable for treating environmental pollutants as well as for water splitting.展开更多
The composition, characteristics and preparation of ionic liquids are presented. The factors influencing the stability of gasoline and the significance of improving gasoline stability are discussed. A novel way to imp...The composition, characteristics and preparation of ionic liquids are presented. The factors influencing the stability of gasoline and the significance of improving gasoline stability are discussed. A novel way to improve the stability of gasoline by using ionic liquid catalyst is developed. The contents of olefin, basic nitrogen and sulfur in gasoline are determined and the optimal experimental conditions for improving gasoline stability are established.The ionic liquid catalyst, which is environmentally friendly, can reduce the olefin content in gasoline, and such process is noted for mild reaction conditions, simple operation, short reaction time, easy recycling of the ionic liquid catalyst and ready separation of products and catalyst.展开更多
The strontium modified waste FCC catalyst was prepared by magnetic stirring method and characterized by Xray diffractometry(XRD),UV-Vis diffuse reflectance spectrometry(DRS),X-ray photoelectron spectroscopy(XPS)and sc...The strontium modified waste FCC catalyst was prepared by magnetic stirring method and characterized by Xray diffractometry(XRD),UV-Vis diffuse reflectance spectrometry(DRS),X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM).Meanwhile,its photocatalytic denitrogenation performance was evaluated in terms of its ability to degrade the N-containing simulation oil under visible light.A mixture of strontium nitrate solution(with a concentration of 0.5 mol/L)and waste FCC catalyst was calcined at 400℃for 5 h prior to taking part in the photocatalytic denitrogenation reaction.The test results showed that the photocatalytic degradation rate of pyridine contained in simulation oil in the presence of the strontium modified FCC catalyst could reach 92.0% under visible light irradiation for 2.5 h.展开更多
Visible-light-driven ZnGaNO solid solution–carbon nitride intercalation compound(CNIC) composite photocatalyst was synthesized via a mixing and heating method. The composite photocatalyst was characterized by X-ray d...Visible-light-driven ZnGaNO solid solution–carbon nitride intercalation compound(CNIC) composite photocatalyst was synthesized via a mixing and heating method. The composite photocatalyst was characterized by X-ray diffraction(XRD), field-emission scanning electron microscopy(FESEM), high-resolution transmission electron microscopy(HRTEM), Fourier transform infrared(FT-IR) spectroscopy, UV-vis diffuse reflection spectroscopy, X-ray photoelectron spectroscopy(XPS), photoluminescence(PL) spectroscopy and BET surface area measurements. The activity of ZnGaNO–CNIC composite photocatalyst for photodegradation of methyl orange(MO) is higher than that of either single-phase CNIC or ZnGaNO solid solution. The as-prepared composite photocatalysts exhibit an improved photocatalytic activity due to enhancement for the separation and transport of photo-generated electron–hole pairs.展开更多
The development of nitrogen-rich biomass- derived carbon catalysts provides an attractive perspective to substitute for Pt-based electrocatalysts for oxygen reduction reaction (ORR). We here report a facile strategy...The development of nitrogen-rich biomass- derived carbon catalysts provides an attractive perspective to substitute for Pt-based electrocatalysts for oxygen reduction reaction (ORR). We here report a facile strategy for synthesis of a nitrogen-doped biocarbon/graphene-like composite electrocatalyst by pyrolyzing a solid-state mixture of coprinus comatus biomass and melamine under nitrogen protection. The graphtic carbon nitride formed by polycondensation of melamine at 600 ℃ acts as a self-sacrificing template to generate the nitrogen-doped graphene-like sheet, which can function as an inserting agent and self-generating support. The composite catalyst exhibits the most promising catalytic activity towards the four-electron ORR with a half-wave potential of around 0.83 V (vs. RHE), and more excellent stability and tolerance to methanol/ethanol compared to the commercial Pt/C catalyst. It is interestingly found that both a higher content of nitrogen and a larger ratio of graphitic-nitrogen species, which may derive from self-addition of graphene-like support into the catalyst, can effectively improve theelectrocatalytic activity. The planar N group may be the nitrogen functionality that is most responsible for main-taining the ORR activity in alkaline medium. This study can largely encourage the exploration of high-performance carbon-based catalysts from economical and sustainable fungus biomass.展开更多
基金supported by the National High Technology Research and Development Program of China (863 Program,2015AA03A401)the National Natural Science Foundation of China (51276039)+1 种基金the Fundamental Research Funds for the Central Universities (020514380020,020514380030)the Postdoctoral Science Foundation of Jiangsu Province,China (1501033A)~~
文摘A series of Fe‐Mn/Al2O3 catalysts were prepared and studied for low temperature selective catalytic reduction (SCR) of NO with NH3 in a fixed‐bed reactor. The effects of Fe and Mn on NO conversion and the deactivation of the catalysts were studied. N2 adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, H2 temperature‐programmed reduction, NH3 temperature‐programmed desorption, X‐ray photoelectron spectroscopy (XPS), thermal gravimetric analysis and Fourier transform infrared spectroscopy were used to character‐ize the catalysts. The 8Fe‐8Mn/Al2O3 catalyst gave 99%of NO conversion at 150?? and more than 92.6%NO conversion was obtained in a wide low temperature range of 90–210??. XPS analysis demonstrated that the Fe3+was the main iron valence state on the catalyst surface and the addition of Mn increased the accumulation of Fe on the surface. The higher specific surface area, enhanced dispersion of amorphous Fe and Mn, improved reduction properties and surface acidity, lower binding energy, higher Mn4+/Mn3+ratio and more adsorbed oxygen species resulted in higher NO conversion for the 8Fe‐8Mn/Al2O3 catalyst. In addition, the SCR activity of the 8Fe‐8Mn/Al2O3 cata‐lyst was only slightly decreased in the presence of H2O and SO2, which indicated that the catalyst had better tolerance to H2O and SO2. The reaction temperature was crucial for the SO2 resistance of catalyst and the decrease of catalytic activity caused by SO2 was mainly due to the sulfate salts formed on the catalyst.
基金supported by the National Basic Research Program of Chain(973 Program,2015CB932300)the National Natural Science Foundation of China(21373175,21321062,21361140374)Fundamental Research Funds for the Central Universities(20720150109)
文摘Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high catalyst loadings required. In the present work, mesoporous Fe/N/C was syn- thesized through heat treatment of K]600 carbon black coated with poly-2-aminobenzimidazole and FeC13. The as-prepared Fe/N/C possesses a unique hollow-shell structure that contains a buffer zone allowing both water formation and vaporization, and also facilitates the mass transfer of gas- eous oxygen. This catalyst generated an oxygen reduction reaction activiW of 9.21 A/g in conjunc- tion with a peak power density of 0.71 W/cm2.
基金supported by the National Natural Science Foundation of China (21476229, 21376236, 21503264)~~
文摘N2O is a promising green propellant and exhibits great potential for satellite propulsion systems. It is difficult for catalytic decomposition, which is an important way to initiate the propulsion process, to occur at temperatures below 600 °C due to the high activation energy of N2O. In this work, we report an Ir supported on rutile TiO2(Ir/r-TiO2) catalyst which exhibits a fairly high activity for high-concentration N2O decomposition. HAADF-STEM, H2-TPR, and XPS results indicate that highly dispersed Ir particles and improved oxygen mobility on the Ir/r-TiO2 could facilitate the decompo-sition of N2O and desorption of the adsorbed oxygen. Bridge-bonded peroxide intermediates were observed with in-situ DRIFT and herein, a detailed decomposition route is proposed.
文摘Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations.Upon tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade.Despite substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied.Herein,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity.Finally,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are provided.In particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.
文摘Normal photocatalysts cannot effectively remove low-concentration NO because of the high recombination rate of the photogenerated carriers.To overcome this problem,S-scheme composites have been developed to fabricate photocatalysts.Herein,a novel S-scheme Sb2WO6/g-C3N4 nanocomposite was fabricated by an ultrasound-assisted method,which exhibited excellent performance for photocatalytic ppb-level NO removal.Compared with the pure constituents of the nanocomposite,the as-prepared 15%-Sb2WO6/g-C3N4 photocatalyst could remove more than 68%continuous-flowing NO(initial concentration:400 ppb)under visible-light irradiation in 30 min.The findings of the trapping experiments confirmed that•O2^–and h+were the important active species in the NO oxidation reaction.Meanwhile,the transient photocurrent response and PL spectroscopy analyses proved that the unique S-scheme structure of the samples could enhance the charge separation efficiency.In situ DRIFTS revealed that the photocatalytic reaction pathway of NO removal over the Sb2WO6/g-C3N4 nanocomposite occurred via an oxygen-induced route.The present work proposes a new concept for fabricating efficient photocatalysts for photocatalytic ppb-level NO oxidation and provides deeper insights into the mechanism of photocatalytic NO oxidation.
基金support from the National Natural Science Foundation of China(51602297 and U1510109)Major Research Project of Shandong Province(2016ZDJS11A04)+3 种基金Fundamental Research Funds for the Central Universities(201612007)Postdoctoral Innovation Program of Shandong Province(201603043)Australia Research Council(ARC)under the Project DP160104089Start-up Foundation for Advanced Talents of Qingdao University of Science and Technology(010022919)~~
文摘A heterojunction photocatalyst based on porous tubular g-C3N4 decorated with CdS nanoparticles was fabricated by a facile hydrothermal co-deposition method.The one-dimensional porous structure of g-C3N4 provides a higher specific surface area,enhanced light absorption,and better separation and transport performance of charge carriers along the longitudinal direction,all of which synergistically contribute to the superior photocatalytic activity observed.The significantly enhanced catalytic efficiency is also a benefit originating from the fast transfer of photogenerated electrons and holes between g-C3N4 and CdS through a built-in electric field,which was confirmed by investigating the morphology,structure,optical properties,electrochemical properties,and photocatalytic activities.Photocatalytic degradation of rhodamine B(RhB)and photocatalytic hydrogen evolution reaction were also carried out to investigate its photocatalytic performance.RhB can be degraded completely within 60 min,and the optimum H2 evolution rate of tubular g-C3N4/CdS composite is as high as 71.6μmol h^–1,which is about 16.3 times higher than that of pure bulk g-C3N4.The as-prepared nanostructure would be suitable for treating environmental pollutants as well as for water splitting.
文摘The composition, characteristics and preparation of ionic liquids are presented. The factors influencing the stability of gasoline and the significance of improving gasoline stability are discussed. A novel way to improve the stability of gasoline by using ionic liquid catalyst is developed. The contents of olefin, basic nitrogen and sulfur in gasoline are determined and the optimal experimental conditions for improving gasoline stability are established.The ionic liquid catalyst, which is environmentally friendly, can reduce the olefin content in gasoline, and such process is noted for mild reaction conditions, simple operation, short reaction time, easy recycling of the ionic liquid catalyst and ready separation of products and catalyst.
基金financially supported by the Science and Technology Project of Fujian Province(No.CE0015)the Ningde Normal University Project on Serving the Western Coast to the TW Strait(No.2010H103)the National-level College Students’ Innovative Entrepreneurial Training Plan Project of Fujian Normal University(Nos.201210394005 and 201310394015)
文摘The strontium modified waste FCC catalyst was prepared by magnetic stirring method and characterized by Xray diffractometry(XRD),UV-Vis diffuse reflectance spectrometry(DRS),X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM).Meanwhile,its photocatalytic denitrogenation performance was evaluated in terms of its ability to degrade the N-containing simulation oil under visible light.A mixture of strontium nitrate solution(with a concentration of 0.5 mol/L)and waste FCC catalyst was calcined at 400℃for 5 h prior to taking part in the photocatalytic denitrogenation reaction.The test results showed that the photocatalytic degradation rate of pyridine contained in simulation oil in the presence of the strontium modified FCC catalyst could reach 92.0% under visible light irradiation for 2.5 h.
基金Project(51208102)supported by the National Natural Science Foundation of China
文摘Visible-light-driven ZnGaNO solid solution–carbon nitride intercalation compound(CNIC) composite photocatalyst was synthesized via a mixing and heating method. The composite photocatalyst was characterized by X-ray diffraction(XRD), field-emission scanning electron microscopy(FESEM), high-resolution transmission electron microscopy(HRTEM), Fourier transform infrared(FT-IR) spectroscopy, UV-vis diffuse reflection spectroscopy, X-ray photoelectron spectroscopy(XPS), photoluminescence(PL) spectroscopy and BET surface area measurements. The activity of ZnGaNO–CNIC composite photocatalyst for photodegradation of methyl orange(MO) is higher than that of either single-phase CNIC or ZnGaNO solid solution. The as-prepared composite photocatalysts exhibit an improved photocatalytic activity due to enhancement for the separation and transport of photo-generated electron–hole pairs.
基金supported by the Basic and Frontier Research Program of Chongqing Municipality (cstc2015jcyj A50032, cstc2014jcyj A50038)the Scientific and Technological Research Program of Chongqing Municipal Education Commission (KJ1501118)+1 种基金the Talent Introduction Project of Chongqing University of Arts and Sciences (R2014CJ02)the National Natural Science Foundation of China (21273292)
文摘The development of nitrogen-rich biomass- derived carbon catalysts provides an attractive perspective to substitute for Pt-based electrocatalysts for oxygen reduction reaction (ORR). We here report a facile strategy for synthesis of a nitrogen-doped biocarbon/graphene-like composite electrocatalyst by pyrolyzing a solid-state mixture of coprinus comatus biomass and melamine under nitrogen protection. The graphtic carbon nitride formed by polycondensation of melamine at 600 ℃ acts as a self-sacrificing template to generate the nitrogen-doped graphene-like sheet, which can function as an inserting agent and self-generating support. The composite catalyst exhibits the most promising catalytic activity towards the four-electron ORR with a half-wave potential of around 0.83 V (vs. RHE), and more excellent stability and tolerance to methanol/ethanol compared to the commercial Pt/C catalyst. It is interestingly found that both a higher content of nitrogen and a larger ratio of graphitic-nitrogen species, which may derive from self-addition of graphene-like support into the catalyst, can effectively improve theelectrocatalytic activity. The planar N group may be the nitrogen functionality that is most responsible for main-taining the ORR activity in alkaline medium. This study can largely encourage the exploration of high-performance carbon-based catalysts from economical and sustainable fungus biomass.