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Title: A ship-in-a-bottle strategy to synthesize encapsulated intermetallic nanoparticle catalysts: Exemplified for furfural hydrogenation

In this paper, 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 nanoparticles (NPs) protected by a mesoporous silica (mSiO2) shell by heterogeneous reduction and nucleation of Sn, Pb, or Zn in mSiO2-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@mSiO2. Among the intermetallic NPs, PtSn@mSiO2 exhibits the best performance, requiring only one-tenth of the quantity of Pt used in Pt@mSiO2 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.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [3] ;  [4] ;  [5] ;  [6]
  1. Iowa State Univ., Ames, IA (United States)
  2. Ames Lab., Ames, IA (United States)
  3. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
  4. Univ. of Kansas, Lawrence, KS (United States)
  5. (Feng) [Univ. of Kansas, Lawrence, KS (United States)
  6. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
Publication Date:
OSTI Identifier:
1240740
Report Number(s):
IS-J--8780
Journal ID: ISSN 2155-5435
Grant/Contract Number:
AC02-07CH11358
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 3; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY intermetallic compounds; site isolation; heterogeneous catalysis; core−shell; green chemistry