【作者】 王军；

【导师】 王艳华；

【作者基本信息】 大连理工大学 ， 有机化学， 2014， 硕士

【摘要】 以离子液体ILPEG1000([CH3(OCH2CH2)nN+Et3][CH3S03-],n=22)为稳定剂,通过氢气还原RuCl3·3H20制得ILPEG1000稳定的Ru纳米催化剂。该催化剂与正庚烷、甲苯组成的温控相分离催化体系有“高温混溶,室温分相”特性,即在反应前室温时,下层为含Ru纳米催化剂的ILPEG1000相,上层为含底物和溶剂的有机相,两相互不相溶。当升温至反应温度时,两相体系混溶为均相,反应在均相中进行。反应结束后冷至室温,体系又重新分为两相,简单分相即可达到催化剂与产物分离以及实现催化剂循环使用。将ILPEG1000稳定的Ru纳米催化剂用于α,β-不饱和醛、酮的选择加氢反应中,催化剂显示了很好的催化活性和选择性。以肉桂醛为例,在优化的反应条件下：T=120℃,t=7h,PH2=4MPa,肉桂醛/Ru=250(摩尔比值),肉桂醛转化率为100%,产物氢化肉桂醛的选择性大于99%。催化剂循环使用4次,催化活性基本保持不变,转化数(TON)值为1,223。ILPEG1000稳定的Ru纳米催化剂在炔烃的选择加氢反应中亦具有良好的催化效果,以苯乙炔为例,在优化的反应条件下：T=105℃,t=2h,PH2=1MPa,苯乙炔/Ru=500(摩尔比值),苯乙炔转化率为95%,产物苯乙烯的选择性为94%。催化剂循环使用4次,催化活性基本保持不变,转化数(TON)值为2,195。更多还原

【Abstract】 Ru nanoparticles stabilized by ionic liquids ILPEG1000([CH3(OCH2CH2)nN+Et3][CH3SO3], n=22) were prepared through hydrogen reduction of RuCl3·3H2O. The thermoregulated phase-separable system consisted of ILPEG1000-stabilized Ru nanoparticles and n-heptane、 toluene possesses the thermoregulated phase-transition property, that is to say, at room temperature before reaction, the lower ILPEG1000phase containing Ru nanoparticles and the upper organic phase containing substrate and solvent are immiscible. When the temperature gradually elevates to the reaction temperature, the biphasic system mingle to a single phase and the reaction proceeds in it smoothly. When the temperature decreases to room temperature, the system becomes biphasic again. The product can be separated from the catalyst easily through simple phase separation and the catalyst can be reused again.ILpEG1000-stabilized Ru nanoparticles were used as catalyst in the selective hydrogenation of α,β-unsaturated aldehydes or ketones, the catalyst exhibited highly catalytic activity and selectivity. For the selective hydrogenation of cinnamaldehyde, under the optimal reaction conditions:T=120℃, t=7h, PH2=4MPa, cinnamaldehyde/Ru=250(molar ratio), the conversion of cinnamaldehyde was100%and the selectivity to hydrocinnamaldehyde was more than99%. The catalyst could be reused for4times without evident loss in activity and selectivity. The turnover number (TON) was1,223.ILpEG1000-stabilized Ru nanoparticles were used as catalyst in the selective hydrogenation of alkynes, the catalyst also exhibited good catalytic effect, for the selective hydrogenation of phenylacetylene, under the optimal reaction conditions:T=105℃, t=2h, PH2=1MPa, phenylacetylene/Ru=500(molar ratio), the conversion of phenylacetylene was95%and the selectivity to styrene was94%. The catalyst could be reused for4times without evident loss in activity and selectivity. The turnover number (TON) was2,195.更多还原