Nano-particle Pd/?-Al2O3 monometallic and Pd-Cu/?-Al2O3 bimetall ic catalysts were prepared by solvated metal atom impregnation (SMAI) method. Th e results of XRD measurement indicated that Pd- Cu alloy was formed in ...Nano-particle Pd/?-Al2O3 monometallic and Pd-Cu/?-Al2O3 bimetall ic catalysts were prepared by solvated metal atom impregnation (SMAI) method. Th e results of XRD measurement indicated that Pd- Cu alloy was formed in the bim etallic catalysts and the crystalline particle size of the alloy increased as Cu contents increased with average diameters < 6.0nm for all the samples. XPS and Auger spectra showed that Pd was in zero- valent state, Cu existed mainly in z ero- valent state and partially in monovalent state Cu+. The Pd/?-Al2O3 and Pd-Cu/?-Al2O3 catalysts exhibited higher activity for CO oxidation at low temperature. The activity of Pd-Cu/?-Al2O3 bimetallic catalyst was hig her than that of Pd/?-Al2O3 monometallic catalyst. The Pd-Cu/?-Al2O3 c atalyst with Pd/Cu atomic ratio of 1∶1 showed the highest activity.展开更多
To obtain a novel support with practical value for metallocene catalyst(\%η\%\|C\-5H\-5)TiCl\-3(CpTiCl\-3), poly(styrene\|co\|4\|vinylpyridine)/SiO\-2 nanoscale hybrid material(SrP/SiO\-2) was firstly produced as sup...To obtain a novel support with practical value for metallocene catalyst(\%η\%\|C\-5H\-5)TiCl\-3(CpTiCl\-3), poly(styrene\|co\|4\|vinylpyridine)/SiO\-2 nanoscale hybrid material(SrP/SiO\-2) was firstly produced as support. After pretreatment by methylaluminoxane(MAO), the hybrid materials reacted with CpTiCl\-3. The results from SAXS, SEM and TEM indicated the morphology and structure of organic/inorganic hybrid materials, and the size of inorganic particle in hybrid was nanoscale. The results from IR and XPS showed that there were two possible cationic active species in the hybrid\|supported catalyst, the polymerization results of styrene proved this possibility.展开更多
采用成核-晶化隔离法制备LiAl-CO_(3)-LDHs晶核,在LDHs晶核晶化的过程中引入葡萄糖分子作为碳源,构筑组成和结构可调的LDHs/C型杂化复合前体。通过高温处理,实现前体的结构拓扑转变及无定形碳组分的去除,得到高比表面积的LiAl复合金属...采用成核-晶化隔离法制备LiAl-CO_(3)-LDHs晶核,在LDHs晶核晶化的过程中引入葡萄糖分子作为碳源,构筑组成和结构可调的LDHs/C型杂化复合前体。通过高温处理,实现前体的结构拓扑转变及无定形碳组分的去除,得到高比表面积的LiAl复合金属氧化物型固体碱催化剂。采用XRD、FT-IR、BET、TEM、SEM、CO_(2)-TPD等表征手段对催化剂的组成、结构、织构性能、表面碱性进行了详细研究,并以苯甲醛和氰基乙酸乙酯间的Knoevenagel缩合反应为探针反应系统地研究了催化剂的碱催化性能。研究结果表明,LDHs/C杂化前体制备过程中葡萄糖与金属离子的摩尔比、水热晶化温度以及焙烧温度是影响催化剂活性的主要因素,晶化温度和焙烧温度的提升不利于碱性位的充分暴露。在150℃的水热晶化温度下,葡萄糖与Al 3+的摩尔比为3时的杂化复合前体经500℃焙烧得到的LiAl-MMO-150-3-500固体催化剂比表面积高达229 m 2·g^(-1),苯酚吸附测得催化剂的总碱量为855μmol·g^(-1),对苯甲醛的转化率高达88.21%。展开更多
文摘Nano-particle Pd/?-Al2O3 monometallic and Pd-Cu/?-Al2O3 bimetall ic catalysts were prepared by solvated metal atom impregnation (SMAI) method. Th e results of XRD measurement indicated that Pd- Cu alloy was formed in the bim etallic catalysts and the crystalline particle size of the alloy increased as Cu contents increased with average diameters < 6.0nm for all the samples. XPS and Auger spectra showed that Pd was in zero- valent state, Cu existed mainly in z ero- valent state and partially in monovalent state Cu+. The Pd/?-Al2O3 and Pd-Cu/?-Al2O3 catalysts exhibited higher activity for CO oxidation at low temperature. The activity of Pd-Cu/?-Al2O3 bimetallic catalyst was hig her than that of Pd/?-Al2O3 monometallic catalyst. The Pd-Cu/?-Al2O3 c atalyst with Pd/Cu atomic ratio of 1∶1 showed the highest activity.
文摘To obtain a novel support with practical value for metallocene catalyst(\%η\%\|C\-5H\-5)TiCl\-3(CpTiCl\-3), poly(styrene\|co\|4\|vinylpyridine)/SiO\-2 nanoscale hybrid material(SrP/SiO\-2) was firstly produced as support. After pretreatment by methylaluminoxane(MAO), the hybrid materials reacted with CpTiCl\-3. The results from SAXS, SEM and TEM indicated the morphology and structure of organic/inorganic hybrid materials, and the size of inorganic particle in hybrid was nanoscale. The results from IR and XPS showed that there were two possible cationic active species in the hybrid\|supported catalyst, the polymerization results of styrene proved this possibility.
文摘采用成核-晶化隔离法制备LiAl-CO_(3)-LDHs晶核,在LDHs晶核晶化的过程中引入葡萄糖分子作为碳源,构筑组成和结构可调的LDHs/C型杂化复合前体。通过高温处理,实现前体的结构拓扑转变及无定形碳组分的去除,得到高比表面积的LiAl复合金属氧化物型固体碱催化剂。采用XRD、FT-IR、BET、TEM、SEM、CO_(2)-TPD等表征手段对催化剂的组成、结构、织构性能、表面碱性进行了详细研究,并以苯甲醛和氰基乙酸乙酯间的Knoevenagel缩合反应为探针反应系统地研究了催化剂的碱催化性能。研究结果表明,LDHs/C杂化前体制备过程中葡萄糖与金属离子的摩尔比、水热晶化温度以及焙烧温度是影响催化剂活性的主要因素,晶化温度和焙烧温度的提升不利于碱性位的充分暴露。在150℃的水热晶化温度下,葡萄糖与Al 3+的摩尔比为3时的杂化复合前体经500℃焙烧得到的LiAl-MMO-150-3-500固体催化剂比表面积高达229 m 2·g^(-1),苯酚吸附测得催化剂的总碱量为855μmol·g^(-1),对苯甲醛的转化率高达88.21%。
基金supported by the National Natural Science Foundation of China(91223202)International Science&Technology Cooperation Program of China(2011DFA73410)+1 种基金Tsinghua University Initiative Scientific Research Program,China(20101081907)National Key Basic Research Program of China(973)(2011CB013102)~~
