Potassium promoted iron–zinc catalysts prepared by co-precipitation method(C–Fe–Zn/K),solvothermal method(S–Fe–Zn/K)and hydrothermal method(H–Fe–Zn/K)could selectively convert CO_2to light olefins,respectively....Potassium promoted iron–zinc catalysts prepared by co-precipitation method(C–Fe–Zn/K),solvothermal method(S–Fe–Zn/K)and hydrothermal method(H–Fe–Zn/K)could selectively convert CO_2to light olefins,respectively.The physicochemical properties of the obtained catalysts were determined by SEM,N_2physisorption,XRD,H_2-TPR,CO_2-TPD and XPS measurements.The results demonstrated that preparation methods had great influences on the morphology,phase structures,reduction and adsorption behavior,and hence the catalytic performance of the catalysts.The samples prepared by hydrothermal and co-precipitation method generated small uniform particles and led to lower specific surface area.In contrast,microspheres with larger specific surface area were formed by self-assembly of nanosheets using solvothermal method.ZnFe_2O_4was the only detectable phase in the fresh C–2Fe–1Zn/K,S–3Fe–1Zn/K and S–2Fe–1Zn/K samples.ZnFe_2O_4and ZnO co-existed with increasing Zncontent in S–1Fe–1Zn/K sample,while ZnO and Fe_2O_3could be observed over H–2Fe–1Zn/K sample.All the used samples contained Fe_3O_4,ZnO and Fe_5C_2.The peak intensity of ZnO was strong in the AR-H–2Fe–1Zn/K sample while it was the lowest in the AR-C–2Fe–1Zn/K sample after reaction.The formation of ZnFe_2O_4increased the interaction between iron and zinc for C–2Fe–1Zn/K and S–Fe–Zn/K samples,causing easier reduction of Fe_2O_3to Fe_3O_4.The surface basicity of the sample prepared by co-precipitation method was much more than that of the other two methods.During CO_2hydrogenation,all the catalysts showed good activity and olefin selectivity.The CO selectivity was increased with increasing Zncontent over S–Fe–Zn/K samples.H–2Fe–1Zn/K catalyst preferred to the production of C_5^+hydrocarbons.CO_2conversion of 54.76%and C_2~=–C_4~=contents of 57.38%were obtained on C–2Fe–1Zn/K sample,respectively.展开更多
Crystalline phase is the key factor for catalyst activity. The zirconium modified PCs/γ-Al2O3 samples were prepared through a simple step incipient-wetness impregnation method. The raw materials and samples were char...Crystalline phase is the key factor for catalyst activity. The zirconium modified PCs/γ-Al2O3 samples were prepared through a simple step incipient-wetness impregnation method. The raw materials and samples were characterized by thermogravimetric-differential analysis （TG-DTA）, X-ray diffraction （XRD）, Fourier transform infrared spectroscopy （FT-IR）, temperature-programmed desorption of ammonia and carbon dioxide （NH3- and CO2-TPD）. The effects of calcination temperature and zirconium content on structure, chemical transformation, and acidity-basicity were investigated. Calcination temperature exhibited the major effect on the crystalline phase of samples. The new phase of A10.1Zr0.901.95 was exhibited which was above 650 ℃. In addition, zirconium content was influenced by the acidic and basic properties of the surface. The acidity and basicity of the ZrPCs/γ-Al2O3 sample increased with the increasing of zirconium content.展开更多
CePO4 （in particular, monoclinic CePO4） has been rarely used to make supported catalysts. Herein, monoclinic CeP04 nanoparticles were prepared by calcining hexagonal CePO4 nanomds （prepared by precipitation） in ai...CePO4 （in particular, monoclinic CePO4） has been rarely used to make supported catalysts. Herein, monoclinic CeP04 nanoparticles were prepared by calcining hexagonal CePO4 nanomds （prepared by precipitation） in air at 900 ℃. Monoclinic CePO4 nanowires were prepared by calcining hexagonal CePO4 nanowires （prepared by hydrothermal synthesis at 150 ℃） in air at 900 ℃. Both monoclinic CePO4 materials were used to support Rh2O3 by impregnation using Rh（NO3）3 as a precursor （followed by calcination）. The catalytic performance of Rh2O3/monoclinic CePO4 composite materials in N2O decomposition and CO oxidation was investigated. It was found that Rh2O3 supported on monoclinic CePO4 nanowims was much more active than Rh2O3 supported on monoclinic CePO4 nanoparticles. The stability of catalysts as a function of reaction time on stream was studied in both reactions. The influence of co-fed CO2, O2, and H2O on the catalytic activity in N20 decomposition was also studied. These catalysts were characterized by employing N2 adsorption-desorption, ICP-OES, XRD, TEM, XPS, H2-TPR, O2-TPD, and CO2-TPD. The correlation between physicochemical properties and catalytic properties was discussed.展开更多
A series of Mg Zn Al hydrotalcites like with different Mg/Zn molar ratios are synthesized by co precipitation method and characterized by XRD. The reactions of dehydrogenation or dehydration of isopropanol are carried...A series of Mg Zn Al hydrotalcites like with different Mg/Zn molar ratios are synthesized by co precipitation method and characterized by XRD. The reactions of dehydrogenation or dehydration of isopropanol are carried out using the Mg Zn Al mixed oxides obtained from calcination of Mg Zn Al hydrotalcites like. All of the Mg Zn Al mixed oxides show high catalytic activity on isopropanol dehydrogenation reaction. The acetone selectivity achieves more than 95%. The relation between catalytic activity and basicity of the catalysts is discussed by CO2 TPD technique.展开更多
The purpose of this study is to increase acrolein yield and capability of coking resistance in the reaction of glycerol dehydration to acrolein by assembling metal phosphate supported on HZSM-5 catalyst. The as-prepar...The purpose of this study is to increase acrolein yield and capability of coking resistance in the reaction of glycerol dehydration to acrolein by assembling metal phosphate supported on HZSM-5 catalyst. The as-prepared catalysts were characterized by XRD, SEM, EDS, BET, NH_3-TPD, CO_2-TPD and Py-IR techniques. It was found that metal phosphate species were incorporated into the porous structure of HZSM-5 zeolites, thus influencing the surface and textural physico-chemical properties of the supporters. The alkaline-treated HZSM-5 catalyst promoted the dispersion of phosphate species on the carriers. Moreover, the amount of strong acidity was tremendously improved by adding the different metal hydrophosphates and the catalysts show high catalytic activity. In this present work, the Sn1/4 H_2PO_4/HZSM-5 catalyst exhibited good performance in the catalytic activity and coking resistant ability, which resulted in a high acrolein yield of 83% initially and acrolein yield of 68% after 30 h. The acidity, especially the ratio of strong to weak acid, plays an important role in promoting acrolein yield and stability simultaneously.展开更多
基金Supports by the National Natural Science Foundation of China(21666030,21366025)National First-rate Discipline Construction Project of Ningxia(NXYLXK2017A04)
文摘Potassium promoted iron–zinc catalysts prepared by co-precipitation method(C–Fe–Zn/K),solvothermal method(S–Fe–Zn/K)and hydrothermal method(H–Fe–Zn/K)could selectively convert CO_2to light olefins,respectively.The physicochemical properties of the obtained catalysts were determined by SEM,N_2physisorption,XRD,H_2-TPR,CO_2-TPD and XPS measurements.The results demonstrated that preparation methods had great influences on the morphology,phase structures,reduction and adsorption behavior,and hence the catalytic performance of the catalysts.The samples prepared by hydrothermal and co-precipitation method generated small uniform particles and led to lower specific surface area.In contrast,microspheres with larger specific surface area were formed by self-assembly of nanosheets using solvothermal method.ZnFe_2O_4was the only detectable phase in the fresh C–2Fe–1Zn/K,S–3Fe–1Zn/K and S–2Fe–1Zn/K samples.ZnFe_2O_4and ZnO co-existed with increasing Zncontent in S–1Fe–1Zn/K sample,while ZnO and Fe_2O_3could be observed over H–2Fe–1Zn/K sample.All the used samples contained Fe_3O_4,ZnO and Fe_5C_2.The peak intensity of ZnO was strong in the AR-H–2Fe–1Zn/K sample while it was the lowest in the AR-C–2Fe–1Zn/K sample after reaction.The formation of ZnFe_2O_4increased the interaction between iron and zinc for C–2Fe–1Zn/K and S–Fe–Zn/K samples,causing easier reduction of Fe_2O_3to Fe_3O_4.The surface basicity of the sample prepared by co-precipitation method was much more than that of the other two methods.During CO_2hydrogenation,all the catalysts showed good activity and olefin selectivity.The CO selectivity was increased with increasing Zncontent over S–Fe–Zn/K samples.H–2Fe–1Zn/K catalyst preferred to the production of C_5^+hydrocarbons.CO_2conversion of 54.76%and C_2~=–C_4~=contents of 57.38%were obtained on C–2Fe–1Zn/K sample,respectively.
基金Supported by the CAS/SAFEA International Partnership Program for Creative Research Teams,National Key R&D program(2016YFB0601303)the National Science Fund for Excellent Young Scholars(21422607)
文摘Crystalline phase is the key factor for catalyst activity. The zirconium modified PCs/γ-Al2O3 samples were prepared through a simple step incipient-wetness impregnation method. The raw materials and samples were characterized by thermogravimetric-differential analysis （TG-DTA）, X-ray diffraction （XRD）, Fourier transform infrared spectroscopy （FT-IR）, temperature-programmed desorption of ammonia and carbon dioxide （NH3- and CO2-TPD）. The effects of calcination temperature and zirconium content on structure, chemical transformation, and acidity-basicity were investigated. Calcination temperature exhibited the major effect on the crystalline phase of samples. The new phase of A10.1Zr0.901.95 was exhibited which was above 650 ℃. In addition, zirconium content was influenced by the acidic and basic properties of the surface. The acidity and basicity of the ZrPCs/γ-Al2O3 sample increased with the increasing of zirconium content.
基金Supported by the National Natural Science Foundation of China(21177028,21477022)
文摘CePO4 （in particular, monoclinic CePO4） has been rarely used to make supported catalysts. Herein, monoclinic CeP04 nanoparticles were prepared by calcining hexagonal CePO4 nanomds （prepared by precipitation） in air at 900 ℃. Monoclinic CePO4 nanowires were prepared by calcining hexagonal CePO4 nanowires （prepared by hydrothermal synthesis at 150 ℃） in air at 900 ℃. Both monoclinic CePO4 materials were used to support Rh2O3 by impregnation using Rh（NO3）3 as a precursor （followed by calcination）. The catalytic performance of Rh2O3/monoclinic CePO4 composite materials in N2O decomposition and CO oxidation was investigated. It was found that Rh2O3 supported on monoclinic CePO4 nanowims was much more active than Rh2O3 supported on monoclinic CePO4 nanoparticles. The stability of catalysts as a function of reaction time on stream was studied in both reactions. The influence of co-fed CO2, O2, and H2O on the catalytic activity in N20 decomposition was also studied. These catalysts were characterized by employing N2 adsorption-desorption, ICP-OES, XRD, TEM, XPS, H2-TPR, O2-TPD, and CO2-TPD. The correlation between physicochemical properties and catalytic properties was discussed.
文摘A series of Mg Zn Al hydrotalcites like with different Mg/Zn molar ratios are synthesized by co precipitation method and characterized by XRD. The reactions of dehydrogenation or dehydration of isopropanol are carried out using the Mg Zn Al mixed oxides obtained from calcination of Mg Zn Al hydrotalcites like. All of the Mg Zn Al mixed oxides show high catalytic activity on isopropanol dehydrogenation reaction. The acetone selectivity achieves more than 95%. The relation between catalytic activity and basicity of the catalysts is discussed by CO2 TPD technique.
基金Supported by the National Natural Science Foundation of China(21676288)
文摘The purpose of this study is to increase acrolein yield and capability of coking resistance in the reaction of glycerol dehydration to acrolein by assembling metal phosphate supported on HZSM-5 catalyst. The as-prepared catalysts were characterized by XRD, SEM, EDS, BET, NH_3-TPD, CO_2-TPD and Py-IR techniques. It was found that metal phosphate species were incorporated into the porous structure of HZSM-5 zeolites, thus influencing the surface and textural physico-chemical properties of the supporters. The alkaline-treated HZSM-5 catalyst promoted the dispersion of phosphate species on the carriers. Moreover, the amount of strong acidity was tremendously improved by adding the different metal hydrophosphates and the catalysts show high catalytic activity. In this present work, the Sn1/4 H_2PO_4/HZSM-5 catalyst exhibited good performance in the catalytic activity and coking resistant ability, which resulted in a high acrolein yield of 83% initially and acrolein yield of 68% after 30 h. The acidity, especially the ratio of strong to weak acid, plays an important role in promoting acrolein yield and stability simultaneously.
