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

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Date
2016-01-01
Authors
Maligal-Ganesh, Raghu
Xiao, Chaoxian
Goh, Tian Wei
Wang, Lin-Lin
Gustafson, Jeffrey
Pei, Yuchen
Qi, Zhiyuan
Johnson, Duane
Zhang, Shiran
Tao, Franklin
Huang, Wenyu
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Ames Laboratory
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Chemistry
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Abstract

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.

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Reprinted (adapted) with permission from ACS Catal., 2016, 6 (3), pp 1754–1763. Copyright 2016 American Chemical Society.

Keywords
core-shell, green chemistry, heterogeneous catalysis, intermetallic compounds, site isolation
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