Nanofluidic Trapping of Faceted Colloidal Nanocrystals for Parallel Single-Particle Catalysis
Journal article, 2022
Catalyst activity can depend distinctly on nanoparticle size and shape. Therefore, understanding the structure sensitivity of catalytic reactions is of fundamental and technical importance. Experiments with single-particle resolution, where ensemble-averaging is eliminated, are required to study it. Here, we implement the selective trapping of individual spherical, cubic, and octahedral colloidal Au nanocrystals in 100 parallel nanofluidic channels to determine their activity for fluorescein reduction by sodium borohydride using fluorescence microscopy. As the main result, we identify distinct structure sensitivity of the rate-limiting borohydride oxidation step originating from different edge site abundance on the three particle types, as confirmed by first-principles calculations. This advertises nanofluidic reactors for the study of structure-function correlations in catalysis and identifies nanoparticle shape as a key factor in borohydride-mediated catalytic reactions.
colloidal Au nanocrystals
single nanoparticle catalysis
fluorescence microscopy
nanoparticle trapping
nanofluidics
first-principles calculations
Author
Sune Levin
Chalmers, Biology and Biological Engineering, Chemical Biology
Sarah Lerch
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Astrid Boje
Chalmers, Physics, Chemical Physics
Joachim Fritzsche
Chalmers, Physics, Chemical Physics
Sriram Kesarimangalam
Chalmers, Biology and Biological Engineering, Chemical Biology
Henrik Ström
Norwegian University of Science and Technology (NTNU)
Chalmers, Mechanics and Maritime Sciences (M2), Fluid Dynamics
Kasper Moth-Poulsen
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Spanish National Research Council (CSIC)
Catalan Institution for Research and Advanced Studies
Henrik Sundén
University of Gothenburg
Chalmers, Chemistry and Chemical Engineering, Chemistry and Biochemistry
Anders Hellman
Chalmers, Physics, Chemical Physics
Fredrik Westerlund
Chalmers, Biology and Biological Engineering, Chemical Biology
Christoph Langhammer
Chalmers, Physics, Chemical Physics
ACS Nano
1936-0851 (ISSN) 1936-086X (eISSN)
Vol. 16 9 15206-15214The Sub-10 nm Challenge in Single Particle Catalysis
Swedish Research Council (VR) (2018-00329), 2019-01-01 -- 2024-12-31.
KCK - Kompetenscentrum Katalys 2022-2026
Johnson Matthey (2500123383), 2022-01-01 -- 2026-12-31.
Volvo Group (PO:2435702-000), 2022-01-01 -- 2026-12-31.
Preem (KCK2022-2026), 2022-01-01 -- 2026-12-31.
Umicore Denmark ApS (KCK2022-2026), 2022-01-01 -- 2026-12-31.
Scania AB (Dnr:2021-036543Pnr:52689-1), 2022-01-01 -- 2026-12-31.
Subject Categories (SSIF 2011)
Other Chemistry Topics
Biocatalysis and Enzyme Technology
Organic Chemistry
DOI
10.1021/acsnano.2c06505
PubMed
36054658