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Nanocrystal bilayer for tandem catalysis

Abstract

Supported catalysts are widely used in industry and can be optimized by tuning the composition and interface of the metal nanoparticles and oxide supports. Rational design of metal–metal oxide interfaces in nanostructured catalysts is critical to achieve better reaction activities and selectivities. We introduce here a new class of nanocrystal tandem catalysts that have multiple metal–metal oxide interfaces for the catalysis of sequential reactions. We utilized a nanocrystal bilayer structure formed by assembling platinum and cerium oxide nanocube monolayers of less than 10 nm on a silica substrate. The two distinct metal–metal oxide interfaces, CeO2–Pt and Pt–SiO2, can be used to catalyse two distinct sequential reactions. The CeO2–Pt interface catalysed methanol decomposition to produce CO and H2, which were subsequently used for ethylene hydroformylation catalysed by the nearby Pt–SiO2 interface. Consequently, propanal was produced selectively from methanol and ethylene on the nanocrystal bilayer tandem catalyst. This new concept of nanocrystal tandem catalysis represents a powerful approach towards designing high-performance, multifunctional nanostructured catalysts.

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Figure 1: Assembly process for the preparation of a nanocrystal bilayer ‘tandem catalyst’.
Figure 2: Monolayer films of Pt nanocubes and CeO2 nanocubes and a bilayer film of CeO2–Pt nanocubes observed by TEM.
Figure 3: Nanocrystal bilayers observed by HRTEM and EDX.
Figure 4: MeOH decomposition over Pt–CeO2 and conventional hydroformylation over Pt–SiO2.
Figure 5: Ethylene hydroformylation with MeOH over a tandem catalyst.

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Acknowledgements

This work was supported by the Director, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the US Department of Energy under Contract No. DE-AC02-05CH11231.

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Contributions

Y.Y., C.T., G.S. and P.Y. conceived and designed the experiments. Y.Y., W.H. and C.A. performed the experiments. Z.H., S.H., T.S. and C.A. contributed materials and analysis tools. Y.Y., C.T., W.H. and P.Y. co-wrote the paper. All authors discussed the results and commented on the manuscript.

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Correspondence to Peidong Yang.

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The authors declare no competing financial interests.

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Yamada, Y., Tsung, CK., Huang, W. et al. Nanocrystal bilayer for tandem catalysis. Nature Chem 3, 372–376 (2011). https://doi.org/10.1038/nchem.1018

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