The effects of atmospheres and precursors on MnOx/TiO2 catalysts were studied, which were prepared by the impregnation method and tested for their NOx conversion activity in ammonia selective catalytic reduction (NH3...The effects of atmospheres and precursors on MnOx/TiO2 catalysts were studied, which were prepared by the impregnation method and tested for their NOx conversion activity in ammonia selective catalytic reduction (NH3-SCR) reactions. Results showed that the manganese carbonate (MC) precursor caused mainly Mn2O3, while the manganese nitrate (MN) precursor resulted primarily in MnO2 and the manganese sulfate (MS) precursor was unchanged. The manganese acetate (MA) precursor leaded obtaining a mixture of Mn2O3 and Mn304. NOn conversion decreased in the following order: MA/TiO2 〉 MC/TiO2 〉 MN/TiO2 〉 MS/TiO2 〉 P25, with a calcination temperature of 773 K in air. Catalysts that were prepared by MA and calcined in oxygen performed strong interaction between Ti and Mn, while MnTiO3 was observed. Compared to the catalysts calcined in nitrogen, those calcined in oxygen had larger diameter and smaller surface area and pore. Catalysts that were prepared by MA and calcined in nitrogen tended to gain higher denitration rates than those in air, since they could be prepared with significant specific surface areas. NO., conversion decreased with calcination atmospheres: Nitrogen〉 Air〉 Oxygen. Meanwhile, amorphous Mn2O3 turned into crystalline Mn2O3, when the temperatures increased from 673 to 873 K.展开更多
Precursor decomposition was used for the preparation of VTeO/SBA-15 catalyst for the selective oxidation of propane to acrolein. The catalyst shows a better performance compared with those prepared by conventional imp...Precursor decomposition was used for the preparation of VTeO/SBA-15 catalyst for the selective oxidation of propane to acrolein. The catalyst shows a better performance compared with those prepared by conventional impregnant method. A yield of 9.3% of acrolein was achieved with 2% V loadings at 500 ℃. XRD, N2-adsorption, H2-TPR, Py-IR and XPS measurements were used to unclose the relationship between the structure and performance of the catalyst.展开更多
The effect of the precursor composition of fused iron catalyst on the performance of Fischer-Tropsch synthesis was investigated. XRD, BET and CO2 adsorption experiments were carried out to provide better insight into ...The effect of the precursor composition of fused iron catalyst on the performance of Fischer-Tropsch synthesis was investigated. XRD, BET and CO2 adsorption experiments were carried out to provide better insight into the relationship therein. The results showed that the selectivity of C5+ hydrocarbon products was dependent on the mole ratio of Fe^2+/Fe^3+, which was represented by a hump-shaped curve. Catalysts with precursors containing Fe3O4 phase favored the magnetite spinal formation during F-T reaction, while Fe(1-x)O-based catalysts were more likely to favor the formation and growth of the iron carbide crystals.展开更多
The cobalt precursor affects the catalytic performance of Co/SiO_2 catalyst remarkably. The catalyst prepared from cobalt acetate exhibits excellent activity, stability and resistance to carbon deposition.
Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5(Si/Al ratio = 15) with aqueous solutions of different Cu precursors(CuCl_2, Cu(NO_3)_2, CuSO_4, Cu(CH_3COO)_2, and ammoniacal copper(II) complex ion). After b...Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5(Si/Al ratio = 15) with aqueous solutions of different Cu precursors(CuCl_2, Cu(NO_3)_2, CuSO_4, Cu(CH_3COO)_2, and ammoniacal copper(II) complex ion). After being pretreated in flowing He at 500 ℃ to form active Cu+, these catalysts exhibited quite different activities in catalytic decomposition of N_2O. CZM-AC(II)(prepared by ammoniacal copper(Ⅱ) complex ion) with 9.4 wt% Cu content was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N_2O conversion at 400 ℃.CZM-CA(prepared using Cu(CH_3COO)_2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N_2O conversion at 425 ℃. CZM-CC, CZMCN, and CZM-CS prepared by using Cu Cl_2, Cu(NO_3)_2, or CuSO_4 as the Cu precursor with similar Cu contents(≈ 1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N_2O conversion at 500 ℃.XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples.The superior activity of CZM-AC(Ⅱ) can be attributed to the high contents of total Cu+and dimeric Cu+among these samples. The influence of co-fed O_2 or H_2O on the catalytic performance of typical samples was also studied.展开更多
Two types of small iron clusters supported on γ-Al2O3-RT(dehydroxylated at room temperature) and γ-Al2O3-800 (dehydroxylated at 800 ℃) were prepared by solvated metal atom impregnation (SMAI) techniques. The ...Two types of small iron clusters supported on γ-Al2O3-RT(dehydroxylated at room temperature) and γ-Al2O3-800 (dehydroxylated at 800 ℃) were prepared by solvated metal atom impregnation (SMAI) techniques. The iron atom precursor complex, bis(toluene)iron(0) formed in the metal atom reactor, was impregnated into γ-Al2O3 having different concentrations of surface hydroxyl groups to study the effect of surface hydroxylation on the crucial stage of iron cluster formation. Catalysts prepared in this way were characterized by TEM, Mǒssbauer, and chemisorption measurements, and the results show that higher concentration of surface hydroxyl groups of γ-Al2O3-RT favors the formation of more positively charged supported iron cluster Fen/γ-Al2O3-RT, and the lower concentration of surface hydroxyl groups of γ-Al2O3-800 favors the formation of basically neutral supported iron cluster Fen/γ-Al2O3-800. The measured results also indicate that the higher concentration of surface hydroxyl groups causes the rapid decomposition of precursor complex, bis(toluene)iron(0), and favors the formation of relatively large iron cluster. Consequently, these two types of catalysts show different catalytic properties in Fischer-Tropsch reaction. The catalytic pattern of Fen/γ-Al2O3-RT in F-T reaction is similar to that of the unreduced γ-Fe2O3 and that of Fen/γ-Al2O3-800 is similar to that of the reduced α-Fe2O3.展开更多
基金Funded by the National "Twelfth Five-Year" Plan for Science&Technology Support of China(No.2011BAE29B02))
文摘The effects of atmospheres and precursors on MnOx/TiO2 catalysts were studied, which were prepared by the impregnation method and tested for their NOx conversion activity in ammonia selective catalytic reduction (NH3-SCR) reactions. Results showed that the manganese carbonate (MC) precursor caused mainly Mn2O3, while the manganese nitrate (MN) precursor resulted primarily in MnO2 and the manganese sulfate (MS) precursor was unchanged. The manganese acetate (MA) precursor leaded obtaining a mixture of Mn2O3 and Mn304. NOn conversion decreased in the following order: MA/TiO2 〉 MC/TiO2 〉 MN/TiO2 〉 MS/TiO2 〉 P25, with a calcination temperature of 773 K in air. Catalysts that were prepared by MA and calcined in oxygen performed strong interaction between Ti and Mn, while MnTiO3 was observed. Compared to the catalysts calcined in nitrogen, those calcined in oxygen had larger diameter and smaller surface area and pore. Catalysts that were prepared by MA and calcined in nitrogen tended to gain higher denitration rates than those in air, since they could be prepared with significant specific surface areas. NO., conversion decreased with calcination atmospheres: Nitrogen〉 Air〉 Oxygen. Meanwhile, amorphous Mn2O3 turned into crystalline Mn2O3, when the temperatures increased from 673 to 873 K.
基金Supported by the Ministry of Science and Technology of China(No. 2005CB221408)the National Natural Science Founda-tion of China(Nos. 20423002, 20571061)Key Scientific Project of Fujian Province, China(No. 2005HZ01-3)
文摘Precursor decomposition was used for the preparation of VTeO/SBA-15 catalyst for the selective oxidation of propane to acrolein. The catalyst shows a better performance compared with those prepared by conventional impregnant method. A yield of 9.3% of acrolein was achieved with 2% V loadings at 500 ℃. XRD, N2-adsorption, H2-TPR, Py-IR and XPS measurements were used to unclose the relationship between the structure and performance of the catalyst.
文摘The effect of the precursor composition of fused iron catalyst on the performance of Fischer-Tropsch synthesis was investigated. XRD, BET and CO2 adsorption experiments were carried out to provide better insight into the relationship therein. The results showed that the selectivity of C5+ hydrocarbon products was dependent on the mole ratio of Fe^2+/Fe^3+, which was represented by a hump-shaped curve. Catalysts with precursors containing Fe3O4 phase favored the magnetite spinal formation during F-T reaction, while Fe(1-x)O-based catalysts were more likely to favor the formation and growth of the iron carbide crystals.
文摘The cobalt precursor affects the catalytic performance of Co/SiO_2 catalyst remarkably. The catalyst prepared from cobalt acetate exhibits excellent activity, stability and resistance to carbon deposition.
基金Supported by the National Natural Science Foundation of China(Grant No.21477022)
文摘Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5(Si/Al ratio = 15) with aqueous solutions of different Cu precursors(CuCl_2, Cu(NO_3)_2, CuSO_4, Cu(CH_3COO)_2, and ammoniacal copper(II) complex ion). After being pretreated in flowing He at 500 ℃ to form active Cu+, these catalysts exhibited quite different activities in catalytic decomposition of N_2O. CZM-AC(II)(prepared by ammoniacal copper(Ⅱ) complex ion) with 9.4 wt% Cu content was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N_2O conversion at 400 ℃.CZM-CA(prepared using Cu(CH_3COO)_2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N_2O conversion at 425 ℃. CZM-CC, CZMCN, and CZM-CS prepared by using Cu Cl_2, Cu(NO_3)_2, or CuSO_4 as the Cu precursor with similar Cu contents(≈ 1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N_2O conversion at 500 ℃.XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples.The superior activity of CZM-AC(Ⅱ) can be attributed to the high contents of total Cu+and dimeric Cu+among these samples. The influence of co-fed O_2 or H_2O on the catalytic performance of typical samples was also studied.
文摘Two types of small iron clusters supported on γ-Al2O3-RT(dehydroxylated at room temperature) and γ-Al2O3-800 (dehydroxylated at 800 ℃) were prepared by solvated metal atom impregnation (SMAI) techniques. The iron atom precursor complex, bis(toluene)iron(0) formed in the metal atom reactor, was impregnated into γ-Al2O3 having different concentrations of surface hydroxyl groups to study the effect of surface hydroxylation on the crucial stage of iron cluster formation. Catalysts prepared in this way were characterized by TEM, Mǒssbauer, and chemisorption measurements, and the results show that higher concentration of surface hydroxyl groups of γ-Al2O3-RT favors the formation of more positively charged supported iron cluster Fen/γ-Al2O3-RT, and the lower concentration of surface hydroxyl groups of γ-Al2O3-800 favors the formation of basically neutral supported iron cluster Fen/γ-Al2O3-800. The measured results also indicate that the higher concentration of surface hydroxyl groups causes the rapid decomposition of precursor complex, bis(toluene)iron(0), and favors the formation of relatively large iron cluster. Consequently, these two types of catalysts show different catalytic properties in Fischer-Tropsch reaction. The catalytic pattern of Fen/γ-Al2O3-RT in F-T reaction is similar to that of the unreduced γ-Fe2O3 and that of Fen/γ-Al2O3-800 is similar to that of the reduced α-Fe2O3.