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
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
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
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
In this work, Pd–Cu/γ-Al2O3 is prepared by the impregnation method and investigated for selective oxygenization of cyclopentene to cyclopentanone. A series of bimetallic Pd–Cu/γ-Al2O3 nanocatalysts were prepared a...In this work, Pd–Cu/γ-Al2O3 is prepared by the impregnation method and investigated for selective oxygenization of cyclopentene to cyclopentanone. A series of bimetallic Pd–Cu/γ-Al2O3 nanocatalysts were prepared and the structures characterized by XRD, XPS and TEM. We determined that the obtained Pd–Cu/γ-Al2O3（molar ratio Pd：Cu = 5：1） was an efficient catalyst for the oxygenization of cyclopentene to cyclopentanone with 95% selectivity and 85% conversion（100 °C, 1 MPa initial O2 pressure, 7 h）.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
Fe3O4 catalyst supported on spherical γ-Al2O3 was prepared with and without ultrasonic treatment during the impregnation step,and the heterogeneous catalytic oxidation of dimethoate wastewater was conducted with Fent...Fe3O4 catalyst supported on spherical γ-Al2O3 was prepared with and without ultrasonic treatment during the impregnation step,and the heterogeneous catalytic oxidation of dimethoate wastewater was conducted with Fenton reagent.Then,the physical and chemical properties of the catalysts were analyzed by means of XRD,ICP-AES and SEM,especially the effect of Fe3O4 dispersity on γ-Al2O3.The results showed that the activity of the supported catalysts prepared with ultrasonic treatment for dimethoate was higher than those without ultrasonic treatment and the corresponding degradation rate doubled those of the catalyst obtained by impregnation.The probable cause was that for catalysts prepared with ultrasonic treatment,Fe3O4 was well dispersed on the catalyst surface with small particle size,or existed in non-crystalline amorphous state,and Fe content on the catalyst surface was higher than those without ultrasonic treatment.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.
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 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.
基金financial assistance from the National Natural Science Foundation of China (Nos. 21272050, 21371044, 21472033 and 21571047)
文摘In this work, Pd–Cu/γ-Al2O3 is prepared by the impregnation method and investigated for selective oxygenization of cyclopentene to cyclopentanone. A series of bimetallic Pd–Cu/γ-Al2O3 nanocatalysts were prepared and the structures characterized by XRD, XPS and TEM. We determined that the obtained Pd–Cu/γ-Al2O3（molar ratio Pd：Cu = 5：1） was an efficient catalyst for the oxygenization of cyclopentene to cyclopentanone with 95% selectivity and 85% conversion（100 °C, 1 MPa initial O2 pressure, 7 h）.
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.
文摘Fe3O4 catalyst supported on spherical γ-Al2O3 was prepared with and without ultrasonic treatment during the impregnation step,and the heterogeneous catalytic oxidation of dimethoate wastewater was conducted with Fenton reagent.Then,the physical and chemical properties of the catalysts were analyzed by means of XRD,ICP-AES and SEM,especially the effect of Fe3O4 dispersity on γ-Al2O3.The results showed that the activity of the supported catalysts prepared with ultrasonic treatment for dimethoate was higher than those without ultrasonic treatment and the corresponding degradation rate doubled those of the catalyst obtained by impregnation.The probable cause was that for catalysts prepared with ultrasonic treatment,Fe3O4 was well dispersed on the catalyst surface with small particle size,or existed in non-crystalline amorphous state,and Fe content on the catalyst surface was higher than those without ultrasonic treatment.
