详细信息
SBA-15锚定的钌杂多酸催化剂的合成及其催化正十六烷氧化 ( EI收录)
Ru-polyoxometalates immobilized on SBA-15 as heterogeneous catalysts for n-hexadecane oxidation
文献类型:期刊文献
中文题名:SBA-15锚定的钌杂多酸催化剂的合成及其催化正十六烷氧化
英文题名:Ru-polyoxometalates immobilized on SBA-15 as heterogeneous catalysts for n-hexadecane oxidation
作者:陈立芳[1];曹文荣[1];苗改[1];王翠花[1];方云进[1];漆志文[1]
机构:[1]华东理工大学化工学院,化学工程联合国家重点实验室,上海200237
年份:2013
卷号:64
期号:2
起止页码:547
中文期刊名:化工学报
外文期刊名:CIESC Journal
收录:CSTPCD;;EI(收录号:20131116114728);Scopus;北大核心:【北大核心2011】;CSCD:【CSCD2013_2014】;
基金:国家自然科学基金项目(21006029,21076074);上海市自然科学基金项目(10ZR1407200)~~
语种:中文
中文关键词:烷烃氧化;锚定;SBA-15;多相催化剂;钌杂多酸
外文关键词:n-alkane oxidation; immobilization; SBA-15; heterogeneous catalysis; Ru-polyoxometalates
摘要:利用(3-氨丙基)三乙氧基硅烷(apts)将钌金属杂多酸[X2W20O70(RuY)2]10-(其中,X为锑或铋,Y为苯或对异丙基苯甲烷)固定在介孔的SBA-15上可得到一系列性能优良的SBA-15锚定的钌杂多酸催化剂。采用XRD、N2吸附-脱附实验和FT-IR红外光谱对此类催化剂进行表征,并检测其对正十六烷氧化的催化性能。结果表明,以空气为氧化剂,在无任何溶剂的条件下,该锚定的钌杂多酸催化剂遵循传统的自由基自氧化机理,将正十六烷烃氧化成各种醇类和酮类,显示出优良的催化性能。因此,这类多相催化剂对环境友好的烷烃氧化反应具有较高的应用价值。
The selective oxidation of alkanes as a green process remains a challenging task because of inactive C--H oxidation. Heterogeneous Ru-polyoxometalates catalysts were synthesized by using organo- ruthenium supported heteropolytungstates,[ Sb2 W20 O70 ( RuC6 H6 ) 2]^10^-, [ Bi2 W20 O70 ( RuC6 H6 )2 ]^10^-, [Sb2 W20 O70 ( RuC10 H14 ) 2 ] 10^-, and [ Bi2 W20 O70 ( RuC10 H14 ) 2 ] ^10- anchored on 3-aminopropyltriethoxysilane (apts)-modified mesoporous SBA-15. The catalysts were characterized by X-ray diffraction (XRD), N2- adsorption measurements and Fourier transform infrared reflectance (FT-IR) spectroscopy. The results of these analyses indicated that these catalysts had high surface area, uniform hexagonal channels which were similar to those of SBA-15, and organo-ruthenium supported heteropolytungstates were highly dispersed in the pores of the modified silica. The heterogeneous Ru-polyoxometalates catalysts were used as catalysts for the solvent-free aerobic oxidation of n-hexadecane to alcohols and ketones by using air as the oxidant under ambient conditions. They exhibited exceptionally high catalytic performance through a classical freeradical autoxidation mechanism. Therefore, the catalysts demonstrated the prospect of this type of heterogeneous catalyst for practical applications.
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