In Situ Plasmonic Nanospectroscopy of the CO Oxidation Reaction over Single Pt Nanoparticles
Artikel i vetenskaplig tidskrift, 2019

The ongoing quest to develop single-particle methods for the in situ study of heterogeneous catalysts is driven by the fact that heterogeneity in terms of size, shape, grain structure, and composition is a general feature among nanoparticles in an ensemble. This heterogeneity hampers the generation of a deeper understanding for how these parameters affect catalytic properties. Here we present a solution that in a single benchtop experimental setup combines single-particle plasmonic nanospectroscopy with mass spectrometry for gas phase catalysis under reaction conditions at high temperature. We measure changes in the surface state of polycrystalline platinum model catalyst particles in the 70 nm size range and the corresponding bistable kinetics during the carbon monoxide oxidation reaction via the peak shift of the dark-field scattering spectrum of a closely adjacent plasmonic nanoantenna sensor and compare these changes with the total reaction rate measured by the mass spectrometer from an ensemble of nominally identical particles. We find that the reaction kinetics of simultaneously measured individual Pt model catalysts are dictated by the grain structure and that the superposition of the individual nanoparticle response can account for the significant broadening observed in the corresponding nanoparticle ensemble data. In a wider perspective our work enables in situ plasmonic nanospectroscopy in controlled gas environments at high temperature to investigate the role of the surface state on transition metal catalysts during reaction and of processes such as alloying or surface segregation in situ at the single-nanoparticle level for model catalysts in the few tens to hundreds of nanometer size range.

plasmonic nanospectroscopy

quadrupole mass spectrometry

single particle

CO oxidation

dark-field scattering spectroscopy

single-particle catalysis

bistable kinetics

Författare

Su Liu

Chalmers, Fysik, Kemisk fysik

Arturo Susarrey- Arce

Chalmers, Fysik, Kemisk fysik

Sara Nilsson

Chalmers, Fysik, Kemisk fysik

David Albinsson

Chalmers, Fysik, Kemisk fysik

Lars Hellberg

Chalmers, Fysik, Kemisk fysik

Svetlana Alekseeva

Chalmers, Fysik, Kemisk fysik

Christoph Langhammer

Chalmers, Fysik, Kemisk fysik

ACS Nano

1936-0851 (ISSN) 1936-086X (eISSN)

Vol. 13 5 6090-6100

Plasmonic antennas shine light on the nanoworld

Knut och Alice Wallenbergs Stiftelse, 2013-07-01 -- 2018-06-30.

Ämneskategorier

Annan kemiteknik

Annan kemi

Metallurgi och metalliska material

Infrastruktur

Chalmers materialanalyslaboratorium

DOI

10.1021/acsnano.9b02876

Mer information

Senast uppdaterat

2019-07-15