温控相分离纳米Pd催化α,β-不饱和酮的选择加氢  

Thermoregulated phase-separable Pd nanocatalyst for selective hydrogenation of α, β-unsaturated ketones

作　　者：杜博文 王艳华[1] DU Bowen;WANG Yanhua(School of Chemical Engineering,Dalian University of Technology,Dalian 116023,Liaoning,China)

机构地区：[1]大连理工大学化工学院,辽宁大连116023

出　　处：《精细化工》2021年第9期1848-1852,共5页Fine Chemicals

基　　金：国家自然科学基金(21173031)。

摘　　要：以Pd(OAc)_(2)、[CH_(3)(OCH_(2)CH_(2))_(22)N^(+)Et_(3)][CH_(3)SO_(3)^(–)](ILPEG1000)为原料,制得温控相分离Pd纳米催化剂,对其进行了UV-Vis和TEM表征。常压氢气条件下在α,β-不饱和酮的选择加氢反应中,Pd纳米催化剂显示了优异的催化性能。在最佳的反应条件下[n(查尔酮)∶n(Pd)=500∶1,n(ILPEG1000)∶n(Pd)=100∶1,90℃,20min,p=1.01×10^(5) Pa(H_(2)气球)],查尔酮的转化率和C==C双键加氢产物的选择性均>99%。Pd纳米催化剂易于与产物分离并可以循环使用6次,循环使用6次后转化率和选择性均>99%。转化频率(TOF)可达1470h^(–1),高于目前文献中报道的常压氢气条件下过渡金属纳米催化剂催化查尔酮选择加氢反应的最高值(870 h^(–1))。Thermoregulated phase-separable Pd nanocatalyst was prepared from Pd(OAc)_(2) and [CH_(3)(OCH_(2)CH_(2))_(22)N^(+)Et_(3)][CH_(3)SO_(3)^(-)](ILPEG1000) and characterized by UV-Vis and TEM. The Pd nanocatalyst exhibited excellent catalytic performance in the selective hydrogenation of α, β-unsaturated ketones at atmospheric hydrogen pressure. Under optimized reaction conditions of n(chalcone)∶n(Pd)=500∶1, n(ILPEG1000)∶n(Pd)=100∶1, 90 ℃, 20 min, p=1.01×10^(5) Pa(H_(2) balloon), both conversion rate and hydrogenation selectivity of the C==C bond for chalcone were above 99%. The Pd nanocatalyst could be easily separated from the product and recycled six times with both conversion and selectivity greater than 99%. The turnover frequency(TOF) was up to 1470 h^(–1), which exceeded the maximum value(870 h^(–1)) of selective hydrogenation of chalcone catalyzed by transition metal nanocatalyst under atmospheric hydrogen pressure reported in the literature.

关 键 词：温控相分离催化 纳米粒子 常压 Α Β-不饱和酮 加氢 催化技术 

分 类 号：O622.4[理学—有机化学]