Composition-tuned oxidation levels of Pt–Re bimetallic nanoparticles for the etherification of allylic alcohols
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Chunhua Yan1(
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The catalytic performance of metal nanoparticles is often affected by surface oxidation levels. Instead of post-synthesis oxidation/reduction, we propose an efficient method to modulate the oxidation levels by tuning the composition of bimetallic nanoparticles. Here we report a series of Pt–Re bimetallic nanoparticles synthesized via a facile thermal co-reduction process, with a uniform size of approximately 3 nm. The investigation of the growth of the Pt–Re nanoparticles suggests that the Re atoms were enriched on the surface, as confirmed by X-ray photoelectron spectroscopy. Furthermore, X-ray absorption spectroscopy showed that metallic Re was decreased and high-valency ReOx species were increased in particles with higher Re/Pt ratios. In the etherification of allylic alcohols catalyzed by Pt–Re nanoparticles of different compositions under ambient conditions, particles with higher Re/Pt ratios exhibited significantly better performances. The highest mass activity of Pt–Re bimetallic nanoparticles (127 μmol·g-1·s-1) was more than forty times that of the industrial catalyst CH3ReO3 (3 μmol·g-1·s-1). The catalytically active sites were associated with ReOx and could be tuned by adjusting the Pt ratio.
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Composition-tuned oxidation levels of Pt–Re bimetallic nanoparticles for the etherification of allylic alcohols
), Chunhua Yan1(
)
Abstract
The catalytic performance of metal nanoparticles is often affected by surface oxidation levels. Instead of post-synthesis oxidation/reduction, we propose an efficient method to modulate the oxidation levels by tuning the composition of bimetallic nanoparticles. Here we report a series of Pt–Re bimetallic nanoparticles synthesized via a facile thermal co-reduction process, with a uniform size of approximately 3 nm. The investigation of the growth of the Pt–Re nanoparticles suggests that the Re atoms were enriched on the surface, as confirmed by X-ray photoelectron spectroscopy. Furthermore, X-ray absorption spectroscopy showed that metallic Re was decreased and high-valency ReOx species were increased in particles with higher Re/Pt ratios. In the etherification of allylic alcohols catalyzed by Pt–Re nanoparticles of different compositions under ambient conditions, particles with higher Re/Pt ratios exhibited significantly better performances. The highest mass activity of Pt–Re bimetallic nanoparticles (127 μmol·g-1·s-1) was more than forty times that of the industrial catalyst CH3ReO3 (3 μmol·g-1·s-1). The catalytically active sites were associated with ReOx and could be tuned by adjusting the Pt ratio.
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Acknowledgements
We thank the National Natural Science Foundation of China (Nos. 21461162001, 21025101, 21621061, and 21331001) and the National Basic Research Program of China (No. 2014CB643803) for financial support.
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