期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 49, 页码 58619-58629出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c17925
关键词
photocatalysts; template-directed synthesis; metal-organic frameworks; asymmetric reaction; heterogeneous
资金
- Tianjin Natural Science Foundation [20JCJQJC00170]
- 111 Project [B12015]
By utilizing a homogeneous Ru photocatalyst as a template, a series of isostructural photocatalyst-encapsulating metal-organic frameworks (photocatalyst@MOFs) were fabricated, showcasing high porosity, robustness, and photocatalyst loading for improved catalytic activity and recyclability in organic reactions.
Photocatalysis is a powerful and versatile tool widely applied in the areas of synthesis chemistry. However, most of the photocatalysts currently used are homogeneous catalysts, which inevitably face issues such as product-catalyst separation and recyclability. Addressing this challenge, we utilized a homogeneous Ru photocatalyst as a structure-directing template to fabricate a series of isostructural photocatalyst-encapsulating metal-organic frameworks (photocatalyst@MOFs) with high porosity, robustness, and photocatalyst loading. The regular channels of MOF can disperse the encapsulated photocatalysts, promote the mass transfer of substrates and products, and provide an outstanding substrate confinement effect, thereby dramatically improving the catalytic activity and excellent recyclability toward valuable organic reactions. For instance, the MOF photocatalysts can catalyze the asymmetric Mannich reaction with ketones with high yields and excellent enantioselectivities (up to 99% ee), better than the reported photocatalyst. Significantly, this was the first case that heterogeneous MOF-based photocatalyst can catalyze the asymmetric Mannich reaction without cocatalysts under room temperature and visible light. This work not only explores an avenue to prepare heterogeneous photocatalysts but also broadens the application scope of MOF-based photocatalysts.
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