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Synthetic Strategies for Adding Enantioselectivity to Metal-Based Solid Catalysts Using Cinchonidine As the Chiral Agent
被引:0
|作者:
Weng, Zhihuan
[1
,2
]
Zaera, Francisco
[1
,2
]
机构:
[1] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA
[2] Univ Calif Riverside, UCR Ctr Catalysis, Riverside, CA 92521 USA
来源:
关键词:
ATOMIC LAYER DEPOSITION;
YOLK-SHELL NANOSTRUCTURES;
HETEROGENEOUS CATALYSTS;
ETHYL PYRUVATE;
MODIFIED PLATINUM;
ASYMMETRIC HYDROGENATION;
SELECTIVE HYDROGENATION;
SUBMONOLAYER CONTROL;
SUPPORTED PLATINUM;
MESOPOROUS SILICA;
D O I:
10.1021/acs.jpcc.4c05485
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
A number of synthetic protocols were developed to produce Pt-based catalysts with chiral characteristics, bestowed by cinchonidine (Cd) moieties in a variety of ways. Two general strategies were explored: (1) the tethering of the Cd modifiers, and (2) the creation of confined spaces above the catalytic sites. Tethering of Cd near the Pt nanoparticles (NPs) of Pt/SiO2 or Pt/Al2O3 catalysts could be optimized, mainly by adjusting the Cd/Pt ratio, to match the performance obtained by adding Cd to the reaction mixture in solution for the enantioselective promotion of the hydrogenation of ethyl pyruvate (EtPy). Encapsulating the Cd fragments adsorbed on Pt inside a thin silica shell proved to also be an excellent way to make an all-heterogeneous enantioselective catalyst. Systematically optimizing the diameter of the 1D pores of SBA-15, a silica mesoporous material with a well-defined structure, by growing thin films of various thicknesses using atomic layer deposition (ALD) was shown to improve the enantioselectivity of the addition of thiols to ketones promoted by tethered Cd. Other approaches were shown to be less successful but to nevertheless offer valuable lessons for the design of multifunctional solid catalysts.
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页码:17446 / 17462
页数:17
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