Article

Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures

  • Nature Communications 5, Article number: 3370 (2014)
  • doi:10.1038/ncomms4370
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Abstract

Hydrogen spillover has been studied for several decades, but its nature, catalytic functions and even its existence remain topics of vigorous debate. This is a consequence of the lack of model catalysts that can provide direct evidences of the existence of hydrogen spillover and simplify the catalytic interpretation. Here we use platinum encapsulated in a dense aluminosilicate matrix with controlled diffusional properties and surface hydroxyl concentrations to elucidate the catalytic functions of hydrogen spillover. The catalytic investigation and theoretical modelling show that surface hydroxyls, presumably Brønsted acids, are crucial for utilizing the catalytic functions of hydrogen spillover on the aluminosilicate surface. The catalysts with optimized nanostructure show remarkable activities in hydro-/dehydrogenation, but virtually no activity for hydrogenolysis. This distinct chemoselectivity may be beneficial in industrially important hydroconversions such as propane dehydrogenation to propylene because the undesired hydrogenolysis pathway producing light hydrocarbons of low value (methane and ethane) is greatly suppressed.

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Acknowledgements

SK Innovation actively participated in scientific discussions and supported the research. This work was also supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) (20110011392) and the Advanced Biomass R&D Center (ABC) of Global Frontier Project (ABC-2010-0029799) funded by the Ministry of Education, Science and Technology. EXAFS experiments at PLS were supported in part by MEST and POSTECH.

Author information

Author notes

    • Juhwan Im
    •  & Hyeyoung Shin

    These authors contributed equally to this work

Affiliations

  1. Korea Advanced Institute of Science and Technology, Department of Chemical and Biomolecular Engineering, Daejeon 305-701, Korea

    • Juhwan Im
    • , Haeyoun Jang
    •  & Minkee Choi
  2. Korea Advanced Institute of Science and Technology, Graduate School of Energy, Environment, Water, and Sustainability (EEWS), Daejeon 305-701, Korea

    • Hyeyoung Shin
    •  & Hyungjun Kim

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Contributions

M.C. conceived and designed the experiments. J.I. performed material synthesis and characterizations. J.I. and H.J. carried out catalytic reactions. H.S. and H.K. performed QM-DFT calculations. M.C. and H.K. wrote the manuscript with assistance from J.I. and H.S. All authors discussed the results and commented on the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Minkee Choi.

Supplementary information

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    Supplementary Information

    Supplementary Figures 1-22, Supplementary Tables 1-2 and Supplementary References

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