College of Chemistry and Chemical Engineering Southwest University, Chongqing, 400715, PR. China.
Dalton Trans. 2011 Apr 7;40(13):3325-35. doi: 10.1039/c0dt00786b. Epub 2011 Feb 18.
In this article, we report the synthesis, structure, morphologies, and asymmetric catalytic properties of a series of novel organosoluble zirconium phosphonate nanocomposites and their supported chiral ruthenium catalysts, which have a good organosolubility (0.1-0.5 g mL(-1)) in various solvents and mesoporous, filiform, and layered structures. Due to the organosoluble properties in various organic solvents, the first homogenization of zirconium phosphonate-supported catalyst was realized in the field of catalysis. In the asymmetric hydrogenation of substituted α-ketoesters, enantioselectivities (74.3-84.7% ee) and isolated yields (86.7-93.6%) were higher than the corresponding homogeneous Ru(p-cymene)(S-BINAP)Cl(2) due to the confinement effect caused by the remaining mesopores in the backbone of the zirconium phosphonate. After completing the reaction, the supported catalyst can be readily recovered in quantitative yield by adding cyclohexane and centrifugation, and reused for five consecutive runs without significant loss in catalytic activity.
在本文中，我们报告了一系列新型有机可溶性锆膦酸盐纳米复合材料及其负载的手性钌催化剂的合成、结构、形态和不对称催化性能，它们在各种溶剂中具有良好的有机可溶性（0.1-0.5 g mL(-1))，具有介孔、丝状和层状结构。由于在各种有机溶剂中的有机可溶性，锆膦酸盐负载催化剂的首次均相化在催化领域得以实现。在取代的α-酮酸酯的不对称氢化中，由于锆膦酸盐骨架中残留的介孔引起的限制效应，对映选择性（74.3-84.7%ee）和分离收率（86.7-93.6%）高于相应的均相 Ru(p-cymene)(S-BINAP)Cl(2)。反应完成后，通过加入环己烷和离心，可定量回收负载催化剂，并可在不损失催化活性的情况下连续使用五轮。
