4.8 Article

A Ship-in-a-Bottle Strategy To Synthesize Encapsulated Intermetallic Nanoparticle Catalysts: Exemplified for Furfural Hydrogenation

Journal

ACS CATALYSIS
Volume 6, Issue 3, Pages 1754-1763

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b02281

Keywords

intermetallic compounds; site isolation; heterogeneous catalysis; core-shell; green chemistry

Funding

  1. Ames Laboratory Royalty Funds
  2. Iowa State University
  3. American Chemical Society Petroleum Research Fund
  4. U.S. Department of Energy, Office of Basic Energy Sciences (BES), Materials Science and Engineering Division
  5. Laboratory-Directed Research and Development funds
  6. U.S. Department of Energy by Iowa State University [DE-AC02-07CH11358]

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Intermetallic compounds are garnering increasing attention as efficient catalysts for improved selectivity in chemical processes. Here, using a ship-in-a-bottle strategy, we synthesize single-phase platinum-based intermetallic nano particles (NPs) protected by a mesoporous silica (mSiO(2)) shell by heterogeneous reduction and nucleation of Sn, Pb, or Zn in mSiO(2)-encapsulated Pt NPs. For selective hydrogenation of furfural to furfuryl alcohol, a dramatic increase in activity and selectivity is observed when intermetallic NPs catalysts are used in comparison to Pt@mSiO(2). Among the intermetallic NPs, PtSn@mSiO(2), exhibits the best performance, requiring only one-tenth of the quantity of Pt used in Pt@mSiO(2) for similar activity and near 100% selectivity to furfuryl alcohol. A high temperature oxidation reduction treatment easily reverses any carbon deposition-induced catalyst deactivation. X-ray photoelectron spectroscopy shows the importance of surface composition to the activity, whereas density functional theory calculations reveal that the enhanced selectivity on PtSn compared to Pt is due to the different furfural adsorption configurations on the two surfaces.

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