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Effect of Ti-Si mixed oxide support on gold catalysts for gas-phase epoxidation of propylene

机译:Ti-Si混合氧化物载体对丙烯气相环氧化金催化剂的影响

摘要

Titania-silica mixed oxides prepared by hydrolytic and one-step non-hydrolytic sol-gel routes using TICl4 and SiCl4 as precursors were employed as the gold catalyst supports for gas-phase epoxiclation of propylene in O-2 and H-2. Characterization studies of the supports and catalysts were performed by means of X-ray diffraction, ultraviolet-visible absorption spectroscopy, N-2 adsorption, and high-resolution transmission electron microscopy. The results indicated that the amorphous Ti-Si mixed oxides containing 6%-14% of Ti could be prepared by both sol-gel routes, but those by non-hydrolytic sol-gel afforded higher surface area and significant mesopores. A superior catalytic performance was obtained with the gold catalyst supported on the non-hydrolytic sol-gel Ti-Si mixed oxide containing 10% of Ti. The propylene conversion was 5.7% at the initial 60 min and 3.3% at 240 min of time on stream. The selectivity for propylene oxide was as high as 95%. The influences of aging time for the non-hydrolytic sol-gel and pH value for the Au deposition-precipitation on the performance of the Au catalyst were also discussed.
机译:通过以TICl4和SiCl4为前体通过水解和一步非水解溶胶-凝胶路线制备的二氧化钛-二氧化硅混合氧化物用作金催化剂载体,用于在O-2和H-2中进行丙烯气相环氧环氧化。通过X射线衍射,紫外可见吸收光谱,N-2吸附和高分辨率透射电子显微镜对载体和催化剂进行表征研究。结果表明,通过两种溶胶-凝胶途径均可制备出含6%-14%Ti的非晶态Ti-Si混合氧化物,而采用非水解溶胶-凝胶法则可提供更高的表面积和明显的中孔。将金催化剂负载在含10%Ti的非水解溶胶-凝胶Ti-Si混合氧化物上,可获得优异的催化性能。在开始运行的60分钟时丙烯转化率为5.7%,在运行240分钟时丙烯转化率为3.3%。环氧丙烷的选择性高达95%。还讨论了非水解溶胶-凝胶的老化时间和金沉积沉淀的pH值对金催化剂性能的影响。

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