Shape-selective sieving layers on an oxide catalyst surface

Christian P. Canlas, Junling Lu, Natalie A. Ray, Nicolas A. Grosso-Giordano, Sungsik Lee, Jeffrey W. Elam, Randall E. Winans, Richard P. Van Duyne, Peter C. Stair, Justin M. Notestein

Research output: Contribution to journalArticle

74 Citations (Scopus)

Abstract

New porous materials such as zeolites, metal-organic frameworks and mesostructured oxides are of immense practical utility for gas storage, separations and heterogeneous catalysis. Their extended pore structures enable selective uptake of molecules or can modify the product selectivity (regioselectivity or enantioselectivity) of catalyst sites contained within. However, diffusion within pores can be problematic for biomass and fine chemicals, and not all catalyst classes can be readily synthesized with pores of the correct dimensions. Here, we present a novel approach that adds reactant selectivity to existing, non-porous oxide catalysts by first grafting the catalyst particles with single-molecule sacrificial templates, then partially overcoating the catalyst with a second oxide through atomic layer deposition. This technique is used to create sieving layers of Al 2O 3 (thickness, 0.4-0.7 nm) with 'nanocavities' (2 photocatalyst. The additional layers result in selectivity (up to 9:1) towards less hindered reactants in otherwise unselective, competitive photocatalytic oxidations and transfer hydrogenations.

Original languageEnglish
Pages (from-to)1030-1036
Number of pages7
JournalNature Chemistry
Volume4
Issue number12
DOIs
Publication statusPublished - Dec 2012

Fingerprint

Oxides
Catalyst selectivity
Catalysts
Zeolites
Regioselectivity
Molecules
Atomic layer deposition
Enantioselectivity
Photocatalysts
Pore structure
Catalysis
Hydrogenation
Porous materials
Biomass
Metals
Oxidation

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Cite this

Canlas, C. P., Lu, J., Ray, N. A., Grosso-Giordano, N. A., Lee, S., Elam, J. W., ... Notestein, J. M. (2012). Shape-selective sieving layers on an oxide catalyst surface. Nature Chemistry, 4(12), 1030-1036. https://doi.org/10.1038/nchem.1477

Shape-selective sieving layers on an oxide catalyst surface. / Canlas, Christian P.; Lu, Junling; Ray, Natalie A.; Grosso-Giordano, Nicolas A.; Lee, Sungsik; Elam, Jeffrey W.; Winans, Randall E.; Van Duyne, Richard P.; Stair, Peter C.; Notestein, Justin M.

In: Nature Chemistry, Vol. 4, No. 12, 12.2012, p. 1030-1036.

Research output: Contribution to journalArticle

Canlas, CP, Lu, J, Ray, NA, Grosso-Giordano, NA, Lee, S, Elam, JW, Winans, RE, Van Duyne, RP, Stair, PC & Notestein, JM 2012, 'Shape-selective sieving layers on an oxide catalyst surface', Nature Chemistry, vol. 4, no. 12, pp. 1030-1036. https://doi.org/10.1038/nchem.1477
Canlas CP, Lu J, Ray NA, Grosso-Giordano NA, Lee S, Elam JW et al. Shape-selective sieving layers on an oxide catalyst surface. Nature Chemistry. 2012 Dec;4(12):1030-1036. https://doi.org/10.1038/nchem.1477
Canlas, Christian P. ; Lu, Junling ; Ray, Natalie A. ; Grosso-Giordano, Nicolas A. ; Lee, Sungsik ; Elam, Jeffrey W. ; Winans, Randall E. ; Van Duyne, Richard P. ; Stair, Peter C. ; Notestein, Justin M. / Shape-selective sieving layers on an oxide catalyst surface. In: Nature Chemistry. 2012 ; Vol. 4, No. 12. pp. 1030-1036.
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