摘要
制备了负载型催化剂Ru/ZrO2·xH2O,并用XRD、XPS和TEM对催化剂进行了表征,所制得的催化剂金属钌的平均粒径约为3.8nm.在2MPa和40℃的温和条件下,以水为溶剂时,Ru/ZrO2·xH2O催化喹啉加氢生成1,2,3,4-四氢喹啉的选择性达98.0%,而且表现出较强的抗氮中毒能力,催化剂循环使用性能稳定.对喹啉加氢反应中的催化反应机理进行了探讨.
The highly dispersed supported catalyst (Ru/ZrO2·xH2O) was prepared and characterized by X-ray diff raction, X-ray photoelectron spectroscopy, and transmission electron microsocpy. The results showed that ruthenium was reduced to low oxidation state and the average partical diameter of Ru particles was about 3.8 nm. The catalyst exhibited high activity in hydrogenation of quinoline under the mild reaction conditions, 40 ℃, 2 MPa, quinoline/Ru molar ratio of 250/1 and H2O as solvent. The conversion of quinoline was 98.2% and the selectity of 1,2,3,4- tetrahydroquinoline was 98.0%. The catalyst can be reused for several times. The mechanism of quinoline hydrogenation over Ru/ZrO2·xH2O catalyst was discussed. The coordination of nitrogen atom of quinoline on the surface of ruthenium nanoparticles and the effect of hydrogen bond between OH groups on ZrO2 surface and nitrogen in quinoline were favourable for the desorption of the substrate and products from the surface of catalyst.
出处
《物理化学学报》
SCIE
CAS
CSCD
北大核心
2008年第6期965-970,共6页
Acta Physico-Chimica Sinica
关键词
钌
二氧化锆
负载型催化剂
喹啉
加氢
四氢喹啉
Ruthenium
Zirconia
Supported catalyst
Quinoline
Hydrogenation
Tetrahydroquinoline