Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis
Journal article, 2021

In heterogeneous catalysis research, the reactivity of individual nanofacets of single particles is typically not resolved. We applied in situ field electron microscopy to the apex of a curved rhodium crystal (radius of 650 nanometers), providing high spatial (∼2 nanometers) and time resolution (∼2 milliseconds) of oscillatory catalytic hydrogen oxidation, to image adsorbed species and reaction fronts on the individual facets. Using ionized water as the imaging species, the active sites were directly imaged with field ion microscopy. The catalytic behavior of differently structured nanofacets and the extent of coupling between them were monitored individually. We observed limited interfacet coupling, entrainment, frequency locking, and reconstruction-induced collapse of spatial coupling. The experimental results are backed up by microkinetic modeling of time-dependent oxygen species coverages and oscillation frequencies.

Author

Y. Suchorski

Vienna University of Technology

Johannes Zeininger

Vienna University of Technology

S. Buhr

Vienna University of Technology

M. Raab

Vienna University of Technology

M. Stoger-Pollach

Vienna University of Technology

J. Bernardi

Vienna University of Technology

Henrik Grönbeck

Chalmers, Physics, Chemical Physics

Competence Centre for Catalysis (KCK)

G. Rupprechter

Vienna University of Technology

Science

0036-8075 (ISSN)

Vol. 372 6548 1314-1318

Subject Categories

Inorganic Chemistry

Atom and Molecular Physics and Optics

Other Chemistry Topics

DOI

10.1126/science.abf8107

PubMed

34016741

More information

Latest update

6/29/2021