Operando detection of single nanoparticle activity dynamics inside a model pore catalyst material

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Science Advances  19 Jun 2020:
Vol. 6, no. 25, eaba7678
DOI: 10.1126/sciadv.aba7678


Nanoconfinement in porous catalysts may induce reactant concentration gradients inside the pores due to local conversion. This leads to inefficient active material use since parts of the catalyst may be trapped in an inactive state. Experimentally, these effects remain unstudied due to material complexity and required high spatial resolution. Here, we have nanofabricated quasi–two-dimensional mimics of porous catalysts, which combine the traits of nanofluidics with single particle plasmonics and online mass spectrometry readout. Enabled by single particle resolution at operando conditions during CO oxidation over a Cu model catalyst, we directly visualize reactant concentration gradient formation due to conversion on single Cu nanoparticles inside the “model pore” and how it dynamically controls oxidation state—and, thus, activity—of particles downstream. Our results provide a general framework for single particle catalysis in the gas phase and highlight the importance of single particle approaches for the understanding of complex catalyst materials.

This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

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