Well-dispersed BaSO4 nanoparticles were synthesized in the presence of sodium polyacrylate (PAAS) by a simple precipitation method, with BaCl2 and (NH4)2SO4 as reactants. The different roles performed by PAAS in t...Well-dispersed BaSO4 nanoparticles were synthesized in the presence of sodium polyacrylate (PAAS) by a simple precipitation method, with BaCl2 and (NH4)2SO4 as reactants. The different roles performed by PAAS in the synthesis of BaSO4 nanoparticles were investigated using X-ray diffractometry, Fourier transform infrared spectroscopy, and transmission electron microscopy. The results indicate that the assynthesized BaSO4 nanoparticles were spheres with an average diameter of 30 nm and that their surfaces were affected by the PAAS. Under a typical procedure employed, PAAS reacted with BaCl2 to yield an intermediate, serving as a control releasing agent and separating the nucleation and crystal growth processes of the BaSO4 nuclei. During formation of the BaSO4 nanospheres, the intermediate slowly dissolved and released barium and polyacrylate ions, inhibiting the growth and aggregation of newly formed BaSO4 seeds and resulting in particles of narrow diameter distribution and improved dispersibility. Moreover, these polyacrylate ions further modified the surfaces of the BaSO4 nanoparticles.展开更多
The application of non-noble metal catalysts in the catalytic direct gas-phase epoxidation of propylene with H2and O2to produce propylene oxide is valuable and challenging. The introduction of alkali metal promoters i...The application of non-noble metal catalysts in the catalytic direct gas-phase epoxidation of propylene with H2and O2to produce propylene oxide is valuable and challenging. The introduction of alkali metal promoters is one of the effective methods to improve the catalytic activity of catalysts. Herein, a series of alkali metal(Li, Na, K, Rb, and Cs)-promoted Ni/TS-1 catalysts were prepared to deeply understand the effect of alkali metals on the structure-activity relationship for gas-phase epoxidation of propylene. Among them, the Na-Ni/TS-1 catalyst exhibits the highest catalytic activity(propylene conversion of 7.35% and PO formation rate of 157.9 g h^(-1)kg_(cat)^(-1)) and the best stability(long-term stability exceeding 140 h at 200 ℃). X-ray absorption and photoelectron spectroscopy revealed that the electronic structure of Ni can be tuned by the addition of alkali metal promoters.NH3-TPD-MS, CO_(2)-TPD-MS, and C_(3)H_(6)-TPD-MS results indicate that the acidity of the catalyst can also be adjusted by the introduction of alkali metal, whereas the Na-Ni/TS-1 catalyst exhibits the strongest C_(3)H_(6) adsorption capacity. Thus, the suitable acid-base properties, unique electronic properties of Ni species, and the strongest propylene adsorption capacity resulted in improved propylene gas-phase epoxidation activity of Na-Ni/TS-1 catalyst. This study not only provides a new strategy for the practical application of nickel-based catalysts in the gas-phase epoxidation of propylene but also provides insights into the promoting effect of alkali metals.展开更多
基金supported by the National Natural Science Foundation of China(51172117)the Shandong Natural Science Foundation(ZR2010EM035)the Qingdao Science and Technology Project(10-3-4-4-12-jch)
文摘Well-dispersed BaSO4 nanoparticles were synthesized in the presence of sodium polyacrylate (PAAS) by a simple precipitation method, with BaCl2 and (NH4)2SO4 as reactants. The different roles performed by PAAS in the synthesis of BaSO4 nanoparticles were investigated using X-ray diffractometry, Fourier transform infrared spectroscopy, and transmission electron microscopy. The results indicate that the assynthesized BaSO4 nanoparticles were spheres with an average diameter of 30 nm and that their surfaces were affected by the PAAS. Under a typical procedure employed, PAAS reacted with BaCl2 to yield an intermediate, serving as a control releasing agent and separating the nucleation and crystal growth processes of the BaSO4 nuclei. During formation of the BaSO4 nanospheres, the intermediate slowly dissolved and released barium and polyacrylate ions, inhibiting the growth and aggregation of newly formed BaSO4 seeds and resulting in particles of narrow diameter distribution and improved dispersibility. Moreover, these polyacrylate ions further modified the surfaces of the BaSO4 nanoparticles.
基金supported by the National Key Research and Development Program of China (2022YFE0208300)the National Natural Science Foundation of China (22078354, 22108290)。
文摘The application of non-noble metal catalysts in the catalytic direct gas-phase epoxidation of propylene with H2and O2to produce propylene oxide is valuable and challenging. The introduction of alkali metal promoters is one of the effective methods to improve the catalytic activity of catalysts. Herein, a series of alkali metal(Li, Na, K, Rb, and Cs)-promoted Ni/TS-1 catalysts were prepared to deeply understand the effect of alkali metals on the structure-activity relationship for gas-phase epoxidation of propylene. Among them, the Na-Ni/TS-1 catalyst exhibits the highest catalytic activity(propylene conversion of 7.35% and PO formation rate of 157.9 g h^(-1)kg_(cat)^(-1)) and the best stability(long-term stability exceeding 140 h at 200 ℃). X-ray absorption and photoelectron spectroscopy revealed that the electronic structure of Ni can be tuned by the addition of alkali metal promoters.NH3-TPD-MS, CO_(2)-TPD-MS, and C_(3)H_(6)-TPD-MS results indicate that the acidity of the catalyst can also be adjusted by the introduction of alkali metal, whereas the Na-Ni/TS-1 catalyst exhibits the strongest C_(3)H_(6) adsorption capacity. Thus, the suitable acid-base properties, unique electronic properties of Ni species, and the strongest propylene adsorption capacity resulted in improved propylene gas-phase epoxidation activity of Na-Ni/TS-1 catalyst. This study not only provides a new strategy for the practical application of nickel-based catalysts in the gas-phase epoxidation of propylene but also provides insights into the promoting effect of alkali metals.