Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 38, Pages 42739-42748Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c10814
Keywords
inorganic-organic framework; functionalized materials; heterogeneous catalysis; hollow/porous materials; substrate-selective catalysis
Funding
- National Natural Science Foundation of China [21876069]
- Six Talent Peaks Project in Jiangsu [XCL-018]
- Jiangsu Funds for Distinguished Young Scientists [BK20190045]
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The search for catalysts with a perfect substrate selectivity toward the hydrogenation of nitroarenes is a goal of high importance, which still remains a significant challenge. Here, we designed a new type of catalyst with superior substrate selectivity by combining a space-confined effect and a hydrogen-bonding network, in which metal nanoparticles (MNPs) were confined in hierarchical hollow silica (HHS) with a poly(N-isopropylacry-lamide) (PNIPA) coating. Given the strong induced properties of hydrogen-bond donors and acceptors in the HHS support and PNIPA coating, the as-synthesized catalyst would achieve perfect substrate selectivity for the hydrogenation of various nitroarenes and their mixture by thoroughly impeding the reduction of nitroarenes with any hydroxyl or carboxyl groups, which is typically very difficult to be realized over almost all of the reported supported-metal catalysts. Notably, the hydrogenation of nitroarenes can produce almost quantitative yields of anilines over the as-synthesized catalyst. Furthermore, density functional theory and experimental evidence are also provided for the hierarchical structure of HHS and PNIPA coating associated with substrates to demonstrate how a substrate could have access or be blocked into the confined active centers (MNPs). Therefore, this work would open a new window to design efficient catalysts for a wide variety of substrate-selective catalyses.
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