A ternary composite of TiO2 and a SiO2-Al2O3 aerogel with good photocatalytic activity was prepared by a simple sol-gel method with TiO2 nanoparticles and SiO2-Al2O3 aerogels derived from industrial fly ash.The struct...A ternary composite of TiO2 and a SiO2-Al2O3 aerogel with good photocatalytic activity was prepared by a simple sol-gel method with TiO2 nanoparticles and SiO2-Al2O3 aerogels derived from industrial fly ash.The structural features of the TiO2/SiO2-Al2O3 aerogel composite were investigated by X-ray powder diffraction,Fourier transform infrared spectroscopy,transmission electron microscopy,gas adsorption measurements and diffuse reflectance UV-visible spectroscopy.The optimal conditions for photocatalytic degradation of 2-sec-butyl-4,6-dinitrophenol（DNBP],included an initial DNBP concentration of 0.167 mmol/L at pH = 4.86 with a catalyst concentration of 6 g/L,under visible light irradiation for 5 h.A plausible mechanism is proposed for the photocatalytic degradation of DNBP.Our composite showed higher photocatalytic activity for DNBP degradation than that of pure TiO2.This indicates that this material can serve as an efficient photocatalyst for degradation of hazardous organic pollutants in wastewater.展开更多
An aqueous sol-gel method for the synthesis of γ-Al2O3 supports has been developed for the use in tar reforming applications. It was determined the influences of two different aluminum precursors (aluminum sec-butoxi...An aqueous sol-gel method for the synthesis of γ-Al2O3 supports has been developed for the use in tar reforming applications. It was determined the influences of two different aluminum precursors (aluminum sec-butoxide (Al[OCH(CH3)CH2CH3]3) and aluminum nitrate (Al(NO3)3)) on the textural and crystallographic properties of Al2O3 supports. Only the formation of γ-Al2O3 is aimed in order to use these alumina materials as catalytic supports, because it presents high specific surface area and pore volume values. Additionally, the synthesis of γ-Al2O3 was realized with the use of a functionalized silicon precursor, [3-(2-aminoethylamino)propyl]trimethoxysilane, called EDAS. By the presence of an ethylenediamine group in this molecule, it is possible to chelate metallic ions and to highly increase their dispersion at a molecular level during the synthesis of metallic catalysts supported on alumina, which is an asset for catalytic applications. So it was developed a synthesis sol-gel procedure for the cogelation between the functionalized silicon alkoxide EDAS and alumina precursor. The alumina supports synthesized with Al(NO3)3 as precursor presented higher porous values than the ones obtained with aluminium sec-butoxide precursor. Since nitrate salts are much easier to handle than alkoxides, these observations allowed validating Al(NO3)3 as aluminum source for the future synthesis procedures for metallic catalysts supported on alumina.展开更多
A carbon-based sulfonated catalyst was prepared by direct sulfonation and carbonization （in moderate conditions：200 ＆#176;C, 12 h） of red liquor solids, a by-product of paper-making process. The prepared sulfonate...A carbon-based sulfonated catalyst was prepared by direct sulfonation and carbonization （in moderate conditions：200 ＆#176;C, 12 h） of red liquor solids, a by-product of paper-making process. The prepared sulfonated cata-lyst （SC） had aromatic structure, composed of carbon enriched inner core, and oxygen-containing （SO3H, COOH, OH） groups enriched surface. The SO3H, COOH, OH groups amounted to 0.74 mmol·g^-1, 0.78 mmol·g^-1, 2.18 mmol·g^-1, respectively. The fresh SC showed much higher catalytic activity than that of the traditional solid acid catalysts （strong-acid 732 cation exchange resin, hydrogen type zeolite socony mobile-five （HZSM-5）, sulfated zir-conia） in esterification of oleic acid. SC was deactivated during the reactions, through the mechanisms of leaching of sulfonated species and formation of sulfonate esters. Two regeneration methods were developed, and the catalytic activity can be mostly regenerated by regeneration Method 1 and be fully regenerated by regeneration Method 2, respectively.展开更多
Spinel lithium manganese oxide ion-sieves have been considered the most promising adsorbents to extract Li^+ from brines and sea water.Here,we report a lithium ion-sieve which was successfully loaded onto tubular α-A...Spinel lithium manganese oxide ion-sieves have been considered the most promising adsorbents to extract Li^+ from brines and sea water.Here,we report a lithium ion-sieve which was successfully loaded onto tubular α-Al2 O3 ceramic substrates by dipping crystallization and post-calcination method.The lithium manganese oxide Li4 Mn5 O(12)was first synthesized onto tubular α-Al2 O3 ceramic substrates as the ion-sieve precursor(i.e.L-AA),and the corresponding lithium ion-sieve(i.e.H-AA) was obtained after acid pickling.The chemical and morphological properties of the ion-sieve were confirmed by X-ray diffraction(XRD) and scanning electron microscopy(SEM).Both L-AA and H-AA showed characteristic peaks of α-Al2 O3 and cubic phase Li4 Mn5 O(12) and the peaks representing cubic phase could still exist after pickling.The lithium manganese oxide Li4 Mn5 O(12) could be uniformly loaded not only on the surface of α-Al2 O3 ubstrates but also inside the pores.Moreover,we found that the equilibrium adsorption capacity of H-AA was 22.9 mg·g^-1.After 12 h adsorption,the adsorption balance was reached.After 5 cycles of adsorption,the adsorption capacity of H-AA was 60.88% of the initial adsorption capacity.The process of H-AA adsorption for Li^+correlated with pseudo-second order kinetic model and Langmuir model.Adsorption thermodynamic parameters regarding enthalpy(△N), Gibbs free energy(△G) and entropy(AS) were calculated.For the dynamic adsorptiondesorption process of H-AA,the H-AA exhibited excellent adsorption performance to Li^+ with the Li^+ dynamic adsorption capacity of 9.74 mg·g^-1 and the Mn^2+dissolution loss rate of 0.99%.After 3 dynamic adsorption-desorption cycles,80% of the initial dynamic adsorption capacity was still kept.展开更多
Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated....Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated. The Ni-supported catalysts were characterized by XRD, TPR and XPS. The relationship between the structures and catalytic activities of the catalysts was discussed. The results showed that the catalytic activity and stability of the Ni/ZrO2-CeO2-Al2O3 catalyst was better than those of other catalysts with the highest CH4 conversion, H2/CO and H2/COx ratio at 750 ℃. The catalyst showed a little deactivation along the reaction time during its 72 h on stream with the mean deactivation rate of 0.08%/h. The catalytic performance of the Ni/ZrO2-CeO2-Al2O3 catalyst was also affected by reaction temperature, no2 ： nCH4 molar ratio and nH2O ： nCH4 molar ratio. TPR, XRD and XPS measurements indicated that the formation of ZrO2-CeO2 solid solution could improve the dispersion of NiO, and inhibit the formation of NiAl2O3, and thus significantly promoted the catalytic activity of the Ni/ZrO2-CeO2-Al2O3 catalyst.展开更多
Composite supports CeO2-ZrO2-Al2O3（CZA） and CeO2-ZrO2-Al2O3-La2O3（CZALa） were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and N...Composite supports CeO2-ZrO2-Al2O3（CZA） and CeO2-ZrO2-Al2O3-La2O3（CZALa） were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles （NGVs） operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction （XRD） and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction （H2-TPR） and oxygen storage capacity （OSC） measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.展开更多
A solid superacid catalyst Pt-SO42-/ZrO2-A12O3 for n-pentane isomerization, was prepared by incipient-wetness impregnation. Preparetion conditions, namely, calcination temperature, concentration of sulfuric acid solut...A solid superacid catalyst Pt-SO42-/ZrO2-A12O3 for n-pentane isomerization, was prepared by incipient-wetness impregnation. Preparetion conditions, namely, calcination temperature, concentration of sulfuric acid solution used in impregnation and Al2O3 concentration, were varied to investigate the effects on catalytic performance of Pt-SO42-/ZrO2-A12O3. The results showed that the PtSZA catalyst exhibited excellent catalytic performance for n-pentane isomerization. Under optimized preparation conditions of calcination temperature of 650°C, reaction time for 3 h, concentration of sulfuric acid solution for 0.5 mol/L, 30% of Al2O3 concentration and 0.3% of Pt concentration, the n-pentane conversion and isopentane selectivity of Pt-SO42-/ZrO2-A12O3 could reach up to 62.17% and 91.60%, respectively.展开更多
基金supported by the National Natural Science Foundation of China(21377018)the Natural Science Foundation of Liaoning Province of China(2013020116)the Fundamental Research Funds for the Central Universities(DUT15ZD240)~~
文摘A ternary composite of TiO2 and a SiO2-Al2O3 aerogel with good photocatalytic activity was prepared by a simple sol-gel method with TiO2 nanoparticles and SiO2-Al2O3 aerogels derived from industrial fly ash.The structural features of the TiO2/SiO2-Al2O3 aerogel composite were investigated by X-ray powder diffraction,Fourier transform infrared spectroscopy,transmission electron microscopy,gas adsorption measurements and diffuse reflectance UV-visible spectroscopy.The optimal conditions for photocatalytic degradation of 2-sec-butyl-4,6-dinitrophenol（DNBP],included an initial DNBP concentration of 0.167 mmol/L at pH = 4.86 with a catalyst concentration of 6 g/L,under visible light irradiation for 5 h.A plausible mechanism is proposed for the photocatalytic degradation of DNBP.Our composite showed higher photocatalytic activity for DNBP degradation than that of pure TiO2.This indicates that this material can serve as an efficient photocatalyst for degradation of hazardous organic pollutants in wastewater.
文摘An aqueous sol-gel method for the synthesis of γ-Al2O3 supports has been developed for the use in tar reforming applications. It was determined the influences of two different aluminum precursors (aluminum sec-butoxide (Al[OCH(CH3)CH2CH3]3) and aluminum nitrate (Al(NO3)3)) on the textural and crystallographic properties of Al2O3 supports. Only the formation of γ-Al2O3 is aimed in order to use these alumina materials as catalytic supports, because it presents high specific surface area and pore volume values. Additionally, the synthesis of γ-Al2O3 was realized with the use of a functionalized silicon precursor, [3-(2-aminoethylamino)propyl]trimethoxysilane, called EDAS. By the presence of an ethylenediamine group in this molecule, it is possible to chelate metallic ions and to highly increase their dispersion at a molecular level during the synthesis of metallic catalysts supported on alumina, which is an asset for catalytic applications. So it was developed a synthesis sol-gel procedure for the cogelation between the functionalized silicon alkoxide EDAS and alumina precursor. The alumina supports synthesized with Al(NO3)3 as precursor presented higher porous values than the ones obtained with aluminium sec-butoxide precursor. Since nitrate salts are much easier to handle than alkoxides, these observations allowed validating Al(NO3)3 as aluminum source for the future synthesis procedures for metallic catalysts supported on alumina.
基金Supported by the National Natural Science Foundation of China(21276076)the Fundamental Research Funds for the Central Universities of China(WA1014003)State Key Laboratory of Chemical Engineering(SKL-ChE-10C06)
文摘A carbon-based sulfonated catalyst was prepared by direct sulfonation and carbonization （in moderate conditions：200 ＆#176;C, 12 h） of red liquor solids, a by-product of paper-making process. The prepared sulfonated cata-lyst （SC） had aromatic structure, composed of carbon enriched inner core, and oxygen-containing （SO3H, COOH, OH） groups enriched surface. The SO3H, COOH, OH groups amounted to 0.74 mmol·g^-1, 0.78 mmol·g^-1, 2.18 mmol·g^-1, respectively. The fresh SC showed much higher catalytic activity than that of the traditional solid acid catalysts （strong-acid 732 cation exchange resin, hydrogen type zeolite socony mobile-five （HZSM-5）, sulfated zir-conia） in esterification of oleic acid. SC was deactivated during the reactions, through the mechanisms of leaching of sulfonated species and formation of sulfonate esters. Two regeneration methods were developed, and the catalytic activity can be mostly regenerated by regeneration Method 1 and be fully regenerated by regeneration Method 2, respectively.
基金This work was financially supported by National Key Research and Development Program(2018YFE0203502),ChinaPrimary Research and Development Plan ofJiangsu Province(BE2019117),China and National Students'Platform for Innovation and Entrepreneurship Training(201910291051Z),China.
文摘Spinel lithium manganese oxide ion-sieves have been considered the most promising adsorbents to extract Li^+ from brines and sea water.Here,we report a lithium ion-sieve which was successfully loaded onto tubular α-Al2 O3 ceramic substrates by dipping crystallization and post-calcination method.The lithium manganese oxide Li4 Mn5 O(12)was first synthesized onto tubular α-Al2 O3 ceramic substrates as the ion-sieve precursor(i.e.L-AA),and the corresponding lithium ion-sieve(i.e.H-AA) was obtained after acid pickling.The chemical and morphological properties of the ion-sieve were confirmed by X-ray diffraction(XRD) and scanning electron microscopy(SEM).Both L-AA and H-AA showed characteristic peaks of α-Al2 O3 and cubic phase Li4 Mn5 O(12) and the peaks representing cubic phase could still exist after pickling.The lithium manganese oxide Li4 Mn5 O(12) could be uniformly loaded not only on the surface of α-Al2 O3 ubstrates but also inside the pores.Moreover,we found that the equilibrium adsorption capacity of H-AA was 22.9 mg·g^-1.After 12 h adsorption,the adsorption balance was reached.After 5 cycles of adsorption,the adsorption capacity of H-AA was 60.88% of the initial adsorption capacity.The process of H-AA adsorption for Li^+correlated with pseudo-second order kinetic model and Langmuir model.Adsorption thermodynamic parameters regarding enthalpy(△N), Gibbs free energy(△G) and entropy(AS) were calculated.For the dynamic adsorptiondesorption process of H-AA,the H-AA exhibited excellent adsorption performance to Li^+ with the Li^+ dynamic adsorption capacity of 9.74 mg·g^-1 and the Mn^2+dissolution loss rate of 0.99%.After 3 dynamic adsorption-desorption cycles,80% of the initial dynamic adsorption capacity was still kept.
基金supported by Guangdong Provincial Natural Science Foundation of China(030514)Science and Technology Plan of Guangdong Province of China(2004B33401006)Doctoral Startup Foundation of Guang Dong Pharmaceutical University.
文摘Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated. The Ni-supported catalysts were characterized by XRD, TPR and XPS. The relationship between the structures and catalytic activities of the catalysts was discussed. The results showed that the catalytic activity and stability of the Ni/ZrO2-CeO2-Al2O3 catalyst was better than those of other catalysts with the highest CH4 conversion, H2/CO and H2/COx ratio at 750 ℃. The catalyst showed a little deactivation along the reaction time during its 72 h on stream with the mean deactivation rate of 0.08%/h. The catalytic performance of the Ni/ZrO2-CeO2-Al2O3 catalyst was also affected by reaction temperature, no2 ： nCH4 molar ratio and nH2O ： nCH4 molar ratio. TPR, XRD and XPS measurements indicated that the formation of ZrO2-CeO2 solid solution could improve the dispersion of NiO, and inhibit the formation of NiAl2O3, and thus significantly promoted the catalytic activity of the Ni/ZrO2-CeO2-Al2O3 catalyst.
基金supported by the National Natural Science Foundation of China (No. 20773090, 20803049)the National High Technology Researchand Development Program of China (863 Program, No. 2006AA06Z347)the Specialized Research Fund for the Doctoral Program of Higher Education(20070610026)
文摘Composite supports CeO2-ZrO2-Al2O3（CZA） and CeO2-ZrO2-Al2O3-La2O3（CZALa） were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles （NGVs） operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction （XRD） and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction （H2-TPR） and oxygen storage capacity （OSC） measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.
文摘A solid superacid catalyst Pt-SO42-/ZrO2-A12O3 for n-pentane isomerization, was prepared by incipient-wetness impregnation. Preparetion conditions, namely, calcination temperature, concentration of sulfuric acid solution used in impregnation and Al2O3 concentration, were varied to investigate the effects on catalytic performance of Pt-SO42-/ZrO2-A12O3. The results showed that the PtSZA catalyst exhibited excellent catalytic performance for n-pentane isomerization. Under optimized preparation conditions of calcination temperature of 650°C, reaction time for 3 h, concentration of sulfuric acid solution for 0.5 mol/L, 30% of Al2O3 concentration and 0.3% of Pt concentration, the n-pentane conversion and isopentane selectivity of Pt-SO42-/ZrO2-A12O3 could reach up to 62.17% and 91.60%, respectively.
