期刊
CHEMICAL SCIENCE
卷 8, 期 7, 页码 5126-5131出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7sc00568g
关键词
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资金
- National Natural Science Foundation of China [21690080, 21690084, 21373206, 21522608, 21673228]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020100]
- National Key Projects for Fundamental Research and Development of China [2016YFA0202801]
- BL 14W beamline at the Shanghai Synchrotron Radiation Facility (SSRF)
- NSF [CHE-1465057]
- Arizona State University
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1465057] Funding Source: National Science Foundation
The chemoselective hydrogenation of substituted nitroarenes to form the corresponding functionalized anilines is an important type of reaction in fine chemistry, and the chemoselectivity is critically dependent on the rational design of the catalysts. This reaction has rarely been accomplished over high-loading Pt catalysts due to the formation of Pt crystals. Here, for the first time, we report that alkali metals (Li+, Na+, K+, etc.) can transform the non-selective high loading Pt/FeOx catalyst to a highly chemoselective one. The best result was obtained over a 5% Na-2.16% Pt/FeOx catalyst, which enhanced the chemoselectivity from 66.4% to 97.4% while the activity remained almost unchanged for the probe reaction of 3-nitrostyrene hydrogenation to 3-aminostyrene. Using aberration-corrected HAADF-STEM, in situ XAS, (57) and Fe Mossbauer and DRIFT spectroscopy, the active site of a Pt-O-Na-O-Fe-like species was proposed, which ensures that the Pt centers are isolated and positively charged for the preferential adsorption of the -NO2 group.
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