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

Abstract

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];  [4];  [5]
+ Show Author Affiliations
  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. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1240740
Report Number(s):
IS-J-8780
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 6; Journal Issue: 3; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; intermetallic compounds; site isolation; heterogeneous catalysis; core−shell; green chemistry

Citation Formats

Maligal-Ganesh, Raghu V., Xiao, Chaoxian, Goh, Tian Wei, Wang, Lin -Lin, Gustafson, Jeffrey, Pei, Yuchen, Qi, Zhiyuan, Johnson, Duane D., Zhang, Shiran, Tao, Franklin, and Huang, Wenyu. A ship-in-a-bottle strategy to synthesize encapsulated intermetallic nanoparticle catalysts: Exemplified for furfural hydrogenation. United States: N. p., 2016. Web. doi:10.1021/acscatal.5b02281.
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Maligal-Ganesh, Raghu V., Xiao, Chaoxian, Goh, Tian Wei, Wang, Lin -Lin, Gustafson, Jeffrey, Pei, Yuchen, Qi, Zhiyuan, Johnson, Duane D., Zhang, Shiran, Tao, Franklin, & Huang, Wenyu. A ship-in-a-bottle strategy to synthesize encapsulated intermetallic nanoparticle catalysts: Exemplified for furfural hydrogenation. United States. https://doi.org/10.1021/acscatal.5b02281
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Maligal-Ganesh, Raghu V., Xiao, Chaoxian, Goh, Tian Wei, Wang, Lin -Lin, Gustafson, Jeffrey, Pei, Yuchen, Qi, Zhiyuan, Johnson, Duane D., Zhang, Shiran, Tao, Franklin, and Huang, Wenyu. 2016. "A ship-in-a-bottle strategy to synthesize encapsulated intermetallic nanoparticle catalysts: Exemplified for furfural hydrogenation". United States. https://doi.org/10.1021/acscatal.5b02281. https://www.osti.gov/servlets/purl/1240740.
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@article{osti_1240740,
title = {A ship-in-a-bottle strategy to synthesize encapsulated intermetallic nanoparticle catalysts: Exemplified for furfural hydrogenation},
author = {Maligal-Ganesh, Raghu V. and Xiao, Chaoxian and Goh, Tian Wei and Wang, Lin -Lin and Gustafson, Jeffrey and Pei, Yuchen and Qi, Zhiyuan and Johnson, Duane D. and Zhang, Shiran and Tao, Franklin and Huang, Wenyu},
abstractNote = {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.},
doi = {10.1021/acscatal.5b02281},
url = {https://www.osti.gov/biblio/1240740}, journal = {ACS Catalysis},
issn = {2155-5435},
number = 3,
volume = 6,
place = {United States},
year = {Thu Jan 28 00:00:00 EST 2016},
month = {Thu Jan 28 00:00:00 EST 2016}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acscatal.5b02281
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    Works referencing / citing this record:

    Recent Advances in Catalytic Hydrogenation of Furfural
    journal, September 2019

    The selective hydrogenation of furfural over intermetallic compounds with outstanding catalytic performance
    journal, January 2019

    Continuous Flow Routes toward Designer Metal Nanocatalysts
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    An integrated immobilization strategy manipulates dual active centers to boost enantioselective tandem reactions
    journal, January 2018

    Transition state and product diffusion control by polymer–nanocrystal hybrid catalysts
    journal, August 2019

    Intermetallic compound catalysts: synthetic scheme, structure characterization and catalytic application
    journal, January 2020

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