Oxidative coupling of methane(OCM) was conducted over LaAlO3X catalysts that were prepared by a coprecipitation method using different co-precipitation pH values(X = 6–10). The aim is to investigate the effect of p H...Oxidative coupling of methane(OCM) was conducted over LaAlO3X catalysts that were prepared by a coprecipitation method using different co-precipitation pH values(X = 6–10). The aim is to investigate the effect of p H values on the catalytic activity of La AlO3 catalysts in this reaction. The results showed that the co-precipitation pH value affected greatly on the formation of chemical species of precipitate precursors in the co-precipitation step, leading to different phases of the finally obtained LaAlO3 catalysts.When the co-precipitation pH value increased up to 8, the lanthanum-related phases such as La2 O3 and La(OH)3 were gradually formed as by-products, preventing the formation of LaAlO3 perovskite crystalline structure and facilitating the formation of oxygen vacancies on catalyst surface. However, at pH value of9 or higher, the lanthanum content in the precipitate precursor was increased greatly. Not LaAlO3 perovskite but lanthanum-related phases were developed as main phases, reducing their catalytic activities in this reaction. Among LaAlO3 catalysts, the one prepared at pH = 8 showed the highest C2 yield due to its well-developed oxygen vacancies and electrophilic lattice oxygen. Therefore, the co-precipitation pH value strongly affected the LaAlO3 catalyst activity in OCM reaction. A precious pH control should be required to prepare various perovskite catalysts for the OCM.展开更多
Well-cubic perovskite lanthanum aluminate (LaAlO3) film on (110) silicon substrate was fabricated by sol-gel method with corresponding inorganic salts. Lanthanum acetate and aluminum acetate glacial acetic acid solut...Well-cubic perovskite lanthanum aluminate (LaAlO3) film on (110) silicon substrate was fabricated by sol-gel method with corresponding inorganic salts. Lanthanum acetate and aluminum acetate glacial acetic acid solutions were prepared via ligand exchange starting from lanthanum nitrate hexahydrate and aluminum nitrate hexahydrate after being refluxed. (CH3CO)2O removed nitrates and the crystallized H2O completely, acetylacetone (AcAc) was partially bidentated with metallic ion of the metallic acetates and formed La(OAc)3 (AcAc)x, which were hydrolyzed into La(AcAc)3 (OH)x by ?x ?x adding 10 ml 0.4% methyl cellulose (MCL) solution. The La(AcAc)3 (OH)x, polymerizing and combining with MCL, ?x formed the LaAlO3 sol precursor with heteropolymeric structure and formed film easily. The epitaxial LaAlO3 film on Si(110) substrate was crystallized after being annealed in thermal annealing furnace for 650?750 °C/30 min. The mor- phologies and microstructures were characterized. The refractive index of the LAO film was 1.942 to 2.007; the dielectric constant and the dissipation factors were estimated to be 23?26 and 2.1×10?4 ? 2.4×10?4 respectively.展开更多
We have studied the interracial reactions between amorphous LaAlO3 thin films and Si substrates, using high- resolution transmission electron microscopy and x-ray photoelectron spectroscopy. It has been shown that the...We have studied the interracial reactions between amorphous LaAlO3 thin films and Si substrates, using high- resolution transmission electron microscopy and x-ray photoelectron spectroscopy. It has been shown that the interracial layer between LaAlO3 film and Si substrate chemical states show that the ratio of La 4d3/2 to Al 2p is SiLaxAlyOz. The depth distributions of La, Si and Al of the interfacial layer remains unchanged with the depth compared to that of the LaAlO3 film. Moreover, the Si content, in the interracial layer gradually decreases with increasing thickness of the interracial layer. These results strongly suggest that the Al element is not deficient in the interracial layer, as previously believed, and the formation of a SiLaxAlyOz interracial layer is mainly due to the diffusion of Si from the substrate during the LaAlO3 film deposition. With the understanding of the interracial layer formation, ones can control the interface characteristics to ensure the desired performances of devices using high-k oxides as gate dielectrics.展开更多
基金supported by C1 Gas Refinery Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT&Future Planning(2015M3D3A1A01064908)
文摘Oxidative coupling of methane(OCM) was conducted over LaAlO3X catalysts that were prepared by a coprecipitation method using different co-precipitation pH values(X = 6–10). The aim is to investigate the effect of p H values on the catalytic activity of La AlO3 catalysts in this reaction. The results showed that the co-precipitation pH value affected greatly on the formation of chemical species of precipitate precursors in the co-precipitation step, leading to different phases of the finally obtained LaAlO3 catalysts.When the co-precipitation pH value increased up to 8, the lanthanum-related phases such as La2 O3 and La(OH)3 were gradually formed as by-products, preventing the formation of LaAlO3 perovskite crystalline structure and facilitating the formation of oxygen vacancies on catalyst surface. However, at pH value of9 or higher, the lanthanum content in the precipitate precursor was increased greatly. Not LaAlO3 perovskite but lanthanum-related phases were developed as main phases, reducing their catalytic activities in this reaction. Among LaAlO3 catalysts, the one prepared at pH = 8 showed the highest C2 yield due to its well-developed oxygen vacancies and electrophilic lattice oxygen. Therefore, the co-precipitation pH value strongly affected the LaAlO3 catalyst activity in OCM reaction. A precious pH control should be required to prepare various perovskite catalysts for the OCM.
文摘Well-cubic perovskite lanthanum aluminate (LaAlO3) film on (110) silicon substrate was fabricated by sol-gel method with corresponding inorganic salts. Lanthanum acetate and aluminum acetate glacial acetic acid solutions were prepared via ligand exchange starting from lanthanum nitrate hexahydrate and aluminum nitrate hexahydrate after being refluxed. (CH3CO)2O removed nitrates and the crystallized H2O completely, acetylacetone (AcAc) was partially bidentated with metallic ion of the metallic acetates and formed La(OAc)3 (AcAc)x, which were hydrolyzed into La(AcAc)3 (OH)x by ?x ?x adding 10 ml 0.4% methyl cellulose (MCL) solution. The La(AcAc)3 (OH)x, polymerizing and combining with MCL, ?x formed the LaAlO3 sol precursor with heteropolymeric structure and formed film easily. The epitaxial LaAlO3 film on Si(110) substrate was crystallized after being annealed in thermal annealing furnace for 650?750 °C/30 min. The mor- phologies and microstructures were characterized. The refractive index of the LAO film was 1.942 to 2.007; the dielectric constant and the dissipation factors were estimated to be 23?26 and 2.1×10?4 ? 2.4×10?4 respectively.
文摘We have studied the interracial reactions between amorphous LaAlO3 thin films and Si substrates, using high- resolution transmission electron microscopy and x-ray photoelectron spectroscopy. It has been shown that the interracial layer between LaAlO3 film and Si substrate chemical states show that the ratio of La 4d3/2 to Al 2p is SiLaxAlyOz. The depth distributions of La, Si and Al of the interfacial layer remains unchanged with the depth compared to that of the LaAlO3 film. Moreover, the Si content, in the interracial layer gradually decreases with increasing thickness of the interracial layer. These results strongly suggest that the Al element is not deficient in the interracial layer, as previously believed, and the formation of a SiLaxAlyOz interracial layer is mainly due to the diffusion of Si from the substrate during the LaAlO3 film deposition. With the understanding of the interracial layer formation, ones can control the interface characteristics to ensure the desired performances of devices using high-k oxides as gate dielectrics.
