A novel powder catalyst Cu-Cr-O applied to the synthesis of carbon nanotubes (CNTs) was developed, which was prepared via ammonia precipitation method. Techniques of thermo-gravimetric/ differential scanning calorim...A novel powder catalyst Cu-Cr-O applied to the synthesis of carbon nanotubes (CNTs) was developed, which was prepared via ammonia precipitation method. Techniques of thermo-gravimetric/ differential scanning calorimeter (TG-DSC), X-ray diffraction (XRD) as well as scanning electron microscopy (SEM) and transmission electron microscopy (TEM) have been employed to characterize the thermal decomposition procedure, crystal phase and micro structural morphologies of the as-synthesized materials, respectively. The results show that carbon nanotubes are successfully synthesized using Cu-Cr-O as catalyst when the precursors are calcined at 400, 500, 600, and 700 ℃. The results indicate that the calcination of the Cu-Cr-O catalyst at 600 ℃ is an effective method to get MWCNT with few nano-tube defects or amorphous carbons.展开更多
Simulated compounds were prepared by loading K2SO4 onto V2O5/AC catalysts. Study the effect of K2SO4 on V1/AC catalysts in the presence of low concentration SO2. Transient response techniques, TPD was carried out. The...Simulated compounds were prepared by loading K2SO4 onto V2O5/AC catalysts. Study the effect of K2SO4 on V1/AC catalysts in the presence of low concentration SO2. Transient response techniques, TPD was carried out. The results indicated that the DeNO activity of V1/AC catalysts was decreased seriously in the early period of operation, but the deactivation was gradually diminished with SO2 adsorption and then, it was completely eliminated. For the sulphated catalysts (saturated catalysts by sulphate), their SCR activity were free from existence of gaseous SO2. the loss of activity about 10% caused by K2SO4 was found on them. The deactivation of K2SO4 deposited catalysts was due to the decrease of adsorbed and activated NH3, or some acid sites.展开更多
Catalyst enhanced chemical vapor deposition of nickel film on high Tg polymers such as teflon(PTFE), polyimide(PI), and polysulfone(PS) was investigated by hot wall and cold wall CVD, in which Ni(dmg)_2, Ni(acac)_2, N...Catalyst enhanced chemical vapor deposition of nickel film on high Tg polymers such as teflon(PTFE), polyimide(PI), and polysulfone(PS) was investigated by hot wall and cold wall CVD, in which Ni(dmg)_2, Ni(acac)_2, Ni(hfac)_2, Ni(TMHD)_2, and Ni(cp)_2 are used as precursors, and palladium complexes are used as catalysts. The films obtained were shiny with silvery color. The Ni was metallic and the purity of Ni was about 92%-95% from XPS analysis. SEM micrographs show that the film had good morphology. The conductivity of the film was about 0.5-4 W·cm^(-1). Ni films had good adhesion with polyimide and polysulfone.展开更多
Platinum, palladium and their alloy films on polyimide were formed by catalyst-enhanced chemical vapor deposition (CVD) in the carrier gas (N2, O2) at 220-300℃ under reduced pressure and normal pressure. The depo...Platinum, palladium and their alloy films on polyimide were formed by catalyst-enhanced chemical vapor deposition (CVD) in the carrier gas (N2, O2) at 220-300℃ under reduced pressure and normal pressure. The deposition of palladium complexes [ Pd((η3-allyl)(hfac) and Pd(hfac)2 ] gives pure palladium film, while the deposition of platinum needs the enhancement of palladium complex by mixing precursor platinum complex Pt(COD)Me2 and palladium complex in the same chamber. The co-deposition of Pd and Pt metals was used for the deposition of alloy films. During the CVD of palladium-platinum alloy, the Pd/Pt atomic ratios vary under different co-deposition conditions. These metal films were characterized by XPS and SEM, and show a good adhesive property.展开更多
The Co Mg O and Co Mn Mg O catalysts are prepared by a co-precipitation method and used as the catalysts for the synthesis of carbon nanotubes(CNTs) through the catalytic chemical vapor deposition(CCVD). The effec...The Co Mg O and Co Mn Mg O catalysts are prepared by a co-precipitation method and used as the catalysts for the synthesis of carbon nanotubes(CNTs) through the catalytic chemical vapor deposition(CCVD). The effects of Mn addition on the carbon yield and structure are investigated. The catalysts are characterized by temperature programmed reduction(TPR) and X-ray diffraction(XRD) techniques, and the synthesized carbon materials are characterized by transmission electron microscopy(TEM) and thermo gravimetric analysis(TG). TEM measurement indicates that the catalyst Co Mg O enclosed completely in the produced graphite layer results in the deactivation of the catalyst. TG results suggest that the Co Mn Mg O catalyst has a higher selectivity for CNTs than Co Mg O. Meanwhile, different diameters of CNTs are synthesized by Co Mn Mg O catalysts with various amounts of Co content, and the results show that the addition of Mn avoids forming the enclosed catalyst, prevents the formation of amorphous carbon, subsequently promotes the growth of CNTs, and the catalyst with decreased Co content is favorable for the synthesis of CNTs with a narrow diameter distribution.The Co Mn Mg O catalyst with 40% Co content has superior catalytic activity for the growth of carbon nanotubes.展开更多
The addition of small amounts of ceria to Co/Al2O3 catalysts increases the turnover rate of the catalyst and C5+ selectivity in the Fischer-Tropsch synthesis. In this work, the amounts of ceria, the calcination tempe...The addition of small amounts of ceria to Co/Al2O3 catalysts increases the turnover rate of the catalyst and C5+ selectivity in the Fischer-Tropsch synthesis. In this work, the amounts of ceria, the calcination temperature, the temperature-programmed reduction (TPR), the temperature-programmed oxidation (TPO), and XRD are investigated. The results show that the addition of small amounts of ceria to Co/Al2O3 catalyst (Ce/Co≈1∶ 10 ~1∶ 7, atom) can increase the CO conversion and liquid yield, while the calcination temperature can control both the chain growth probability and CO conversion in a reverse trend. The TPR and TPO experiments show that small amounts of Ceria can improve the reducibility, but the amounts of carbon deposit increase, and two-type carbon deposition is found in the short-term reaction catalyst.展开更多
Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigate...Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigated. The catalytic combustion of HCHO was considered as the probe reaction for comparing the catalyst activity. The BET, X-ray diffraction, X-ray photoelectron spectroscopy (XPS), and reduction (TPR) were carried out to analyze the influence factor on the catalysts activity. The results showed that the addition of dispersant and use of microwave in the support preparation procedure could be beneficial for enhancing the interaction of supports and gold species and thus improved the catalytic activity. The total conversion temperature for HCHO was 146 ℃ over AC400. With the modification during supports preparation process, the catalytic activity increased with total conversion temperature decreasing to 98 ℃. The results of XPS indicated that Au^0 and Au^+1 species coexisted in these catalysts and the activity of catalyst correlated with Au^+1/Au^0 ratio. Temperature-programmed reduction results demonstrated that the reduction peak appeared between 100-170 ℃ with the inducing of gold. The dependence of activity on the reduction peak temperature implied that ionic gold was catalytic activity component for HCHO oxidation.展开更多
The effects of carbon dioxide content on the catalytic performance and coke formation of nickel catalyst supported on mesoporous nanocrystalline zirconia with high surface area and pure tetragonal crystalline phase we...The effects of carbon dioxide content on the catalytic performance and coke formation of nickel catalyst supported on mesoporous nanocrystalline zirconia with high surface area and pure tetragonal crystalline phase were investigated in methane reforming with carbon dioxide. The samples were characterized by XRD, BET, TPR, TPO, TPH, TEM, and SEM techniques. The catalyst prepared showed high surface area and a mesoporous structure with a narrow pore size distribution. The obtained results revealed that the increase in CO2 content increased the methane conversion and stability of the catalyst and significantly reduced the coke deposition. The TPH analysis showed that several species of carbon with different reactivities toward hydrogenation were deposited on the spent catalysts employed under different CO2 contents.展开更多
FeCo-Al2O3 catalyst was prepared by an ultrasonic coprecipitation (UC) method for the growth of carbon nanotubes (CNTs) from catalytic decomposition of methane.Its catalytic performance was compared with that of t...FeCo-Al2O3 catalyst was prepared by an ultrasonic coprecipitation (UC) method for the growth of carbon nanotubes (CNTs) from catalytic decomposition of methane.Its catalytic performance was compared with that of the FeCo-Al2O3 catalyst counterparts prepared by stepwise impregnation (I) and conventional coprecipitation (C) methods,respectively.The structure and properties of the catalysts and the CNTs as produced thereon were investigated by means of XRD,XPS,TEM and N2 adsorption techniques.It was found that the catalyst prepared by the ultrasonic coprecipitation method was more active,and the yield and purity of the synthesized CNTs were promoted evidently.The XPS results revealed that there were more active components on the surface of the catalyst prepared by the ultrasonic coprecipitation method.On the other hand,N2 adsorption demonstrated that the catalyst prepared by the ultrasonic coprecipitation method conferred larger specific surface area,which was beneficial to dispersion of active components.TEM images further confirmed its higher dispersion.These factors could be responsible for its higher activity for the growth of CNTs from catalytic decomposition of methane.展开更多
To have uniform nanoparticles individually dispersed on substrate before single-walled carbon nanotubes(SWNTs)growth at high temperature is the key for controlling the diameter of the SWNTs.In this letter,a facile app...To have uniform nanoparticles individually dispersed on substrate before single-walled carbon nanotubes(SWNTs)growth at high temperature is the key for controlling the diameter of the SWNTs.In this letter,a facile approach to control the diameter and distribution of the SWNTs by improving the dispersion of the uniform Fe/Mo nanoparticles on silicon wafers with silica layer chemically modified by 1,1,1,3,3,3-hexamethyldisilazane under different conditions is reported.It is found that the dispersion of the catalyst nanoparticles on Si wafer surface can be improved greatly from hydrophilic to hydrophobic,and the diameter and distribution of the SWNTs depend strongly on the dispersion of the catalyst on the substrate surface.Well dispersion of the catalyst results in relatively smaller diameter and narrower distribution of the SWNTs due to the decrease of aggregation and enhancement of dispersion of the catalyst nanoparticles before growth.It is also found that the diameter of the superlong aligned SWNTs is smaller with more narrow distribution than that of random nanotubes.展开更多
A series of LaAl 1-xFe xO 3 catalysts prepared with lanthanum nitrate, aluminium nitrate and iron nitrate was investigated in catalytical syntheses of carbon nanotubes with high yields and purity. The properties ...A series of LaAl 1-xFe xO 3 catalysts prepared with lanthanum nitrate, aluminium nitrate and iron nitrate was investigated in catalytical syntheses of carbon nanotubes with high yields and purity. The properties of carbon nanotubes prepared by the method of CVD(chemical vapor deposition) with n-hexane as the carbon resource were studied and it was shown that the diameter of carbon nanotubes can be controlled by the molar ratio of iron to aluminum in the catalysts and that the diameter of carbon nanotubes changes a little with the decrease of the iron content in the catalysts. From the TEM pictures of carbon nanotubes, it can be found that the LaAl 1-xFe xO 3 catalysts have a significant influence on the wall thickness of the carbon nanotubes, whereas they have little influence on the inner diameter of the carbon nanotubes.展开更多
The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via...The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al2O3 catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al2O3 supports were adjusted by calcining the commercial γ-Al2O3 at different temperatures(600–1200 C). CO methanation reaction was carried out in the temperature range of 300–600 C at different weight hourly space velocities(WHSV = 30000 and 120000 mL·g-1h-1) and pressures(0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al2O3 supports due to the rapid decrease of the specific surface area and acidity of Al2O3 supports. Interestingly, Ni catalysts supported on Al2O3 calcined at 1200 C(Ni/Al2O3-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al2O3-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures(600, 800 and 1000 C). These findings would therefore be helpful to develop Ni/Al2O3 methanation catalyst for SNG production.展开更多
Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared usin...Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared using multiple characterization methods. Pore blockage and active site coverage caused by chlorine-containing organics are responsible for catalyst deactivation. The reactions of chloroethylene and acetylene with chlorine free radical can generate chlorine-containing organic species. SiO_2 and functional groups on activated carbon contribute to the generation of carbon deposition. No significant reduction in the total content of mercury was observed after catalyst deactivation, while there was mercury loss locally. The irreversible loss of HgCl_2 caused by volatilization, reduction and poisoning of elements S and P also can lead to catalyst deactivation. Si, Al, Ca and Fe oxides are scattered on the activated carbon. Active components are still uniformly absorbed on activated carbon after catalyst deactivation.展开更多
Straight carbon nanotubes (CNTs) were achieved by simple thermal chemical vapor deposition(STCVD) catalyzed by Mo-Fe alloy catalyst on silica supporting substrate at 700℃. High-resolution transmission electron micros...Straight carbon nanotubes (CNTs) were achieved by simple thermal chemical vapor deposition(STCVD) catalyzed by Mo-Fe alloy catalyst on silica supporting substrate at 700℃. High-resolution transmission electron microscopy images show that the straight CNTs are well graphitized with no attached amorphous carbon. Mo-Fe alloy catalyst particles play a very crucial role in the growth of straight CNTs. The straight carbon nanotubes contain much less defects than the curved nanotubes and might have potential applications for nanoelectrical devices in the future. The simple synthesis of straight CNTs may have benefit for large-scale productions.展开更多
Alumina-supported bimetallic cobalt-nickel catalyst has been prepared and employed in a fixed-bed reactor for the direct production of synthesis gas from glycerol steam reforming. Physicochemical properties of the 5Co...Alumina-supported bimetallic cobalt-nickel catalyst has been prepared and employed in a fixed-bed reactor for the direct production of synthesis gas from glycerol steam reforming. Physicochemical properties of the 5Co-10Ni/85Al2O3 catalyst were determined from N2-physisorption, H2-chemisorption, CO2 and NH3-temperature-programmed desorption measurements as well as X-ray diffraction analysis. Both weak and strong acid sites are present on the catalyst surface. The acidic:basic ratio is about 7. Carbon deposition was evident at 923 K;addition of H2 however has managed to reduce the carbon deposition. Significantly, this has resulted in the increment of CH4 formation rate, consistent with the increased carbon gasification and methanation. Carbon deposition was almost non-existent, particularly at 1023 K. In addition, the inclusion of hydrogen also has contributed to the decrease of CO2 and increase of CO formation rates. This was attributed to the reverse water-gas-shift reaction. Overall, both the CO2:CO and CO2:CH4 ratios decrease with the hydrogen partial pressure.展开更多
The synthesis of carbon nanotubes (CNTs) via chemical vapour deposition of methane on NiO/γ-Al2O3 catalyst has been investigated.The reduction behavior of NiO/γ-Al2O3 by methane was studied using thermogravimetric...The synthesis of carbon nanotubes (CNTs) via chemical vapour deposition of methane on NiO/γ-Al2O3 catalyst has been investigated.The reduction behavior of NiO/γ-Al2O3 by methane was studied using thermogravimetric (TG) and X-ray diffraction (XRD) techniques.It was found that the NiO supported on γ-Al2O3,was reduced to Ni0 in methane atmosphere in the temperature range of 710-770℃.The catalytic activity of NiO/γ-Al2O3 for CNTs synthesis by in situ chemical vapour deposition of methane during the reduction was also investigated.Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to observe the CNTs produced at various reduction temperatures.The results indicated that the reduction temperature exhibits obvious influence on the morphology and the yield of CNTs.CNTs with the diameter of about 20 nm were obtained at reduction temperature of 750℃,and higher reduction temperature (such as 800 and 850℃) led to an increase in CNTs diameter and a decrease in CNTs yield.展开更多
基金Supported by National Natural Science Foundation of China(No.51201107)Key Basic Research Project of Shanghai Committee of Science and Technology in China(10JC1411800)
文摘A novel powder catalyst Cu-Cr-O applied to the synthesis of carbon nanotubes (CNTs) was developed, which was prepared via ammonia precipitation method. Techniques of thermo-gravimetric/ differential scanning calorimeter (TG-DSC), X-ray diffraction (XRD) as well as scanning electron microscopy (SEM) and transmission electron microscopy (TEM) have been employed to characterize the thermal decomposition procedure, crystal phase and micro structural morphologies of the as-synthesized materials, respectively. The results show that carbon nanotubes are successfully synthesized using Cu-Cr-O as catalyst when the precursors are calcined at 400, 500, 600, and 700 ℃. The results indicate that the calcination of the Cu-Cr-O catalyst at 600 ℃ is an effective method to get MWCNT with few nano-tube defects or amorphous carbons.
文摘Simulated compounds were prepared by loading K2SO4 onto V2O5/AC catalysts. Study the effect of K2SO4 on V1/AC catalysts in the presence of low concentration SO2. Transient response techniques, TPD was carried out. The results indicated that the DeNO activity of V1/AC catalysts was decreased seriously in the early period of operation, but the deactivation was gradually diminished with SO2 adsorption and then, it was completely eliminated. For the sulphated catalysts (saturated catalysts by sulphate), their SCR activity were free from existence of gaseous SO2. the loss of activity about 10% caused by K2SO4 was found on them. The deactivation of K2SO4 deposited catalysts was due to the decrease of adsorbed and activated NH3, or some acid sites.
基金Funded by the National Natural Science Foundation of China(51566005)
文摘Catalyst enhanced chemical vapor deposition of nickel film on high Tg polymers such as teflon(PTFE), polyimide(PI), and polysulfone(PS) was investigated by hot wall and cold wall CVD, in which Ni(dmg)_2, Ni(acac)_2, Ni(hfac)_2, Ni(TMHD)_2, and Ni(cp)_2 are used as precursors, and palladium complexes are used as catalysts. The films obtained were shiny with silvery color. The Ni was metallic and the purity of Ni was about 92%-95% from XPS analysis. SEM micrographs show that the film had good morphology. The conductivity of the film was about 0.5-4 W·cm^(-1). Ni films had good adhesion with polyimide and polysulfone.
基金Funded by the National Natural Science Foundation of China (Nos. 20275011 and 20675033)
文摘Platinum, palladium and their alloy films on polyimide were formed by catalyst-enhanced chemical vapor deposition (CVD) in the carrier gas (N2, O2) at 220-300℃ under reduced pressure and normal pressure. The deposition of palladium complexes [ Pd((η3-allyl)(hfac) and Pd(hfac)2 ] gives pure palladium film, while the deposition of platinum needs the enhancement of palladium complex by mixing precursor platinum complex Pt(COD)Me2 and palladium complex in the same chamber. The co-deposition of Pd and Pt metals was used for the deposition of alloy films. During the CVD of palladium-platinum alloy, the Pd/Pt atomic ratios vary under different co-deposition conditions. These metal films were characterized by XPS and SEM, and show a good adhesive property.
基金Project supported by the National Basic Research Program of China(Grant No.2011CB201202)
文摘The Co Mg O and Co Mn Mg O catalysts are prepared by a co-precipitation method and used as the catalysts for the synthesis of carbon nanotubes(CNTs) through the catalytic chemical vapor deposition(CCVD). The effects of Mn addition on the carbon yield and structure are investigated. The catalysts are characterized by temperature programmed reduction(TPR) and X-ray diffraction(XRD) techniques, and the synthesized carbon materials are characterized by transmission electron microscopy(TEM) and thermo gravimetric analysis(TG). TEM measurement indicates that the catalyst Co Mg O enclosed completely in the produced graphite layer results in the deactivation of the catalyst. TG results suggest that the Co Mn Mg O catalyst has a higher selectivity for CNTs than Co Mg O. Meanwhile, different diameters of CNTs are synthesized by Co Mn Mg O catalysts with various amounts of Co content, and the results show that the addition of Mn avoids forming the enclosed catalyst, prevents the formation of amorphous carbon, subsequently promotes the growth of CNTs, and the catalyst with decreased Co content is favorable for the synthesis of CNTs with a narrow diameter distribution.The Co Mn Mg O catalyst with 40% Co content has superior catalytic activity for the growth of carbon nanotubes.
文摘The addition of small amounts of ceria to Co/Al2O3 catalysts increases the turnover rate of the catalyst and C5+ selectivity in the Fischer-Tropsch synthesis. In this work, the amounts of ceria, the calcination temperature, the temperature-programmed reduction (TPR), the temperature-programmed oxidation (TPO), and XRD are investigated. The results show that the addition of small amounts of ceria to Co/Al2O3 catalyst (Ce/Co≈1∶ 10 ~1∶ 7, atom) can increase the CO conversion and liquid yield, while the calcination temperature can control both the chain growth probability and CO conversion in a reverse trend. The TPR and TPO experiments show that small amounts of Ceria can improve the reducibility, but the amounts of carbon deposit increase, and two-type carbon deposition is found in the short-term reaction catalyst.
基金the National Natural Science Foundation of China (20563003)Natural Science Foundation of Inner Mongolia (200508010203)
文摘Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigated. The catalytic combustion of HCHO was considered as the probe reaction for comparing the catalyst activity. The BET, X-ray diffraction, X-ray photoelectron spectroscopy (XPS), and reduction (TPR) were carried out to analyze the influence factor on the catalysts activity. The results showed that the addition of dispersant and use of microwave in the support preparation procedure could be beneficial for enhancing the interaction of supports and gold species and thus improved the catalytic activity. The total conversion temperature for HCHO was 146 ℃ over AC400. With the modification during supports preparation process, the catalytic activity increased with total conversion temperature decreasing to 98 ℃. The results of XPS indicated that Au^0 and Au^+1 species coexisted in these catalysts and the activity of catalyst correlated with Au^+1/Au^0 ratio. Temperature-programmed reduction results demonstrated that the reduction peak appeared between 100-170 ℃ with the inducing of gold. The dependence of activity on the reduction peak temperature implied that ionic gold was catalytic activity component for HCHO oxidation.
文摘The effects of carbon dioxide content on the catalytic performance and coke formation of nickel catalyst supported on mesoporous nanocrystalline zirconia with high surface area and pure tetragonal crystalline phase were investigated in methane reforming with carbon dioxide. The samples were characterized by XRD, BET, TPR, TPO, TPH, TEM, and SEM techniques. The catalyst prepared showed high surface area and a mesoporous structure with a narrow pore size distribution. The obtained results revealed that the increase in CO2 content increased the methane conversion and stability of the catalyst and significantly reduced the coke deposition. The TPH analysis showed that several species of carbon with different reactivities toward hydrogenation were deposited on the spent catalysts employed under different CO2 contents.
文摘FeCo-Al2O3 catalyst was prepared by an ultrasonic coprecipitation (UC) method for the growth of carbon nanotubes (CNTs) from catalytic decomposition of methane.Its catalytic performance was compared with that of the FeCo-Al2O3 catalyst counterparts prepared by stepwise impregnation (I) and conventional coprecipitation (C) methods,respectively.The structure and properties of the catalysts and the CNTs as produced thereon were investigated by means of XRD,XPS,TEM and N2 adsorption techniques.It was found that the catalyst prepared by the ultrasonic coprecipitation method was more active,and the yield and purity of the synthesized CNTs were promoted evidently.The XPS results revealed that there were more active components on the surface of the catalyst prepared by the ultrasonic coprecipitation method.On the other hand,N2 adsorption demonstrated that the catalyst prepared by the ultrasonic coprecipitation method conferred larger specific surface area,which was beneficial to dispersion of active components.TEM images further confirmed its higher dispersion.These factors could be responsible for its higher activity for the growth of CNTs from catalytic decomposition of methane.
基金financial support from NSFC(2117315951420105002)
文摘To have uniform nanoparticles individually dispersed on substrate before single-walled carbon nanotubes(SWNTs)growth at high temperature is the key for controlling the diameter of the SWNTs.In this letter,a facile approach to control the diameter and distribution of the SWNTs by improving the dispersion of the uniform Fe/Mo nanoparticles on silicon wafers with silica layer chemically modified by 1,1,1,3,3,3-hexamethyldisilazane under different conditions is reported.It is found that the dispersion of the catalyst nanoparticles on Si wafer surface can be improved greatly from hydrophilic to hydrophobic,and the diameter and distribution of the SWNTs depend strongly on the dispersion of the catalyst on the substrate surface.Well dispersion of the catalyst results in relatively smaller diameter and narrower distribution of the SWNTs due to the decrease of aggregation and enhancement of dispersion of the catalyst nanoparticles before growth.It is also found that the diameter of the superlong aligned SWNTs is smaller with more narrow distribution than that of random nanotubes.
基金Supported by the Natural Science Foundation of Guangdong Province(No.0 314 2 0 ),the Guangzhou City Science andTechnology Project(No.2 0 0 3Z3- D2 0 71) and the Science and Technology Project of Guangdong Province(No.2 0 0 3C335 0 5
文摘A series of LaAl 1-xFe xO 3 catalysts prepared with lanthanum nitrate, aluminium nitrate and iron nitrate was investigated in catalytical syntheses of carbon nanotubes with high yields and purity. The properties of carbon nanotubes prepared by the method of CVD(chemical vapor deposition) with n-hexane as the carbon resource were studied and it was shown that the diameter of carbon nanotubes can be controlled by the molar ratio of iron to aluminum in the catalysts and that the diameter of carbon nanotubes changes a little with the decrease of the iron content in the catalysts. From the TEM pictures of carbon nanotubes, it can be found that the LaAl 1-xFe xO 3 catalysts have a significant influence on the wall thickness of the carbon nanotubes, whereas they have little influence on the inner diameter of the carbon nanotubes.
基金supported by the Hundred Talents Program of the Chinese Academy of Sciences (CAS),State Key Laboratory of Multiphase Complex Systems of China (No.MPCS-2009-C-01)the National Key Technology R&D Program of China (No.2010BAC66B01)the Knowledge Innovation Program of the CAS (No.KGCX2-YW-396)
文摘The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al2O3 catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al2O3 supports were adjusted by calcining the commercial γ-Al2O3 at different temperatures(600–1200 C). CO methanation reaction was carried out in the temperature range of 300–600 C at different weight hourly space velocities(WHSV = 30000 and 120000 mL·g-1h-1) and pressures(0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al2O3 supports due to the rapid decrease of the specific surface area and acidity of Al2O3 supports. Interestingly, Ni catalysts supported on Al2O3 calcined at 1200 C(Ni/Al2O3-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al2O3-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures(600, 800 and 1000 C). These findings would therefore be helpful to develop Ni/Al2O3 methanation catalyst for SNG production.
基金Supported by the National Science Fund for Excellent Young Scholars of China(No.51522405)
文摘Mercury-containing catalysts are widely used for acetylene hydrochlorination in China. Surface chemical characteristics of the fresh low-level mercury catalysts and spent low-level mercury catalysts were compared using multiple characterization methods. Pore blockage and active site coverage caused by chlorine-containing organics are responsible for catalyst deactivation. The reactions of chloroethylene and acetylene with chlorine free radical can generate chlorine-containing organic species. SiO_2 and functional groups on activated carbon contribute to the generation of carbon deposition. No significant reduction in the total content of mercury was observed after catalyst deactivation, while there was mercury loss locally. The irreversible loss of HgCl_2 caused by volatilization, reduction and poisoning of elements S and P also can lead to catalyst deactivation. Si, Al, Ca and Fe oxides are scattered on the activated carbon. Active components are still uniformly absorbed on activated carbon after catalyst deactivation.
基金Project(KM200510772013) supported by the Science and Technology Development Program of Education Committee of Beijing City Project (2005-2007) supported by the Academic Innovative Team Program(Novel Sensor and Materials: Nanodevice and Nanomaterials) of Education Committee of Beijing City
文摘Straight carbon nanotubes (CNTs) were achieved by simple thermal chemical vapor deposition(STCVD) catalyzed by Mo-Fe alloy catalyst on silica supporting substrate at 700℃. High-resolution transmission electron microscopy images show that the straight CNTs are well graphitized with no attached amorphous carbon. Mo-Fe alloy catalyst particles play a very crucial role in the growth of straight CNTs. The straight carbon nanotubes contain much less defects than the curved nanotubes and might have potential applications for nanoelectrical devices in the future. The simple synthesis of straight CNTs may have benefit for large-scale productions.
文摘Alumina-supported bimetallic cobalt-nickel catalyst has been prepared and employed in a fixed-bed reactor for the direct production of synthesis gas from glycerol steam reforming. Physicochemical properties of the 5Co-10Ni/85Al2O3 catalyst were determined from N2-physisorption, H2-chemisorption, CO2 and NH3-temperature-programmed desorption measurements as well as X-ray diffraction analysis. Both weak and strong acid sites are present on the catalyst surface. The acidic:basic ratio is about 7. Carbon deposition was evident at 923 K;addition of H2 however has managed to reduce the carbon deposition. Significantly, this has resulted in the increment of CH4 formation rate, consistent with the increased carbon gasification and methanation. Carbon deposition was almost non-existent, particularly at 1023 K. In addition, the inclusion of hydrogen also has contributed to the decrease of CO2 and increase of CO formation rates. This was attributed to the reverse water-gas-shift reaction. Overall, both the CO2:CO and CO2:CH4 ratios decrease with the hydrogen partial pressure.
基金supported by the Key Project of Chinese Ministry of Education(No. 208076)Foundation for Outstanding Young Scientist in Shandong Province(BS2009CL004)the Open Foundation of Chemical Engineering Subject of Qingdao University of Science & Technology(No. 20100102)
文摘The synthesis of carbon nanotubes (CNTs) via chemical vapour deposition of methane on NiO/γ-Al2O3 catalyst has been investigated.The reduction behavior of NiO/γ-Al2O3 by methane was studied using thermogravimetric (TG) and X-ray diffraction (XRD) techniques.It was found that the NiO supported on γ-Al2O3,was reduced to Ni0 in methane atmosphere in the temperature range of 710-770℃.The catalytic activity of NiO/γ-Al2O3 for CNTs synthesis by in situ chemical vapour deposition of methane during the reduction was also investigated.Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to observe the CNTs produced at various reduction temperatures.The results indicated that the reduction temperature exhibits obvious influence on the morphology and the yield of CNTs.CNTs with the diameter of about 20 nm were obtained at reduction temperature of 750℃,and higher reduction temperature (such as 800 and 850℃) led to an increase in CNTs diameter and a decrease in CNTs yield.