Light-Off in Plasmon-Mediated Photocatalysis
Journal article, 2021

In plasmon-mediated photocatalysis it is of critical importance to differentiate light-induced catalytic reaction rate enhancement channels, which include near-field effects, direct hot carrier injection, and photothermal catalyst heating. In particular, the discrimination of photothermal and hot electron channels is experimentally challenging, and their role is under keen debate. Here we demonstrate using the example of CO oxidation over nanofabricated neat Pd and Au50Pd50 alloy catalysts, how photothermal rate enhancement differs by up to 3 orders of magnitude for the same photon flux, and how this effect is controlled solely by the position of catalyst operation along the light-off curve measured in the dark. This highlights that small fluctuations in reactor temperature or temperature gradients across a sample may dramatically impact global and local photothermal rate enhancement, respectively, and thus control both the balance between different rate enhancement mechanisms and the way strategies to efficiently distinguish between them should be devised.

plasmonics

CO oxidation

photocatalysis

gold-palladium

heterogeneous catalysis

photothermal

nanoalloys

Author

Christopher Tiburski

Chalmers, Physics, Chemical Physics

Astrid Boje

Chalmers, Physics, Chemical Physics

Sara Nilsson

Chalmers, Physics, Chemical Physics

Zafer Say

Chalmers, Physics, Chemical Physics

Joachim Fritzsche

Chalmers, Physics, Chemical Physics

Henrik Ström

Chalmers, Mechanics and Maritime Sciences, Fluid Dynamics

Anders Hellman

Chalmers, Physics, Chemical Physics

Christoph Langhammer

Chalmers, Physics, Chemical Physics

ACS Nano

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

Vol. 15 7 11535-11542

Subject Categories

Chemical Process Engineering

Atom and Molecular Physics and Optics

Other Physics Topics

DOI

10.1021/acsnano.1c01537

PubMed

34156229

More information

Latest update

7/29/2021