Measuring and directing charge transfer in heterogenous catalysts

Michael J. Zachman (), Victor Fung, Felipe Polo-Garzon, Shaohong Cao, Jisue Moon, Zhennan Huang, Jiang De-en, Zili Wu and Miaofang Chi ()
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Michael J. Zachman: Oak Ridge National Laboratory
Victor Fung: Oak Ridge National Laboratory
Felipe Polo-Garzon: Oak Ridge National Laboratory
Shaohong Cao: Oak Ridge National Laboratory
Jisue Moon: Oak Ridge National Laboratory
Zhennan Huang: Oak Ridge National Laboratory
Jiang De-en: University of California
Zili Wu: Oak Ridge National Laboratory
Miaofang Chi: Oak Ridge National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Precise control of charge transfer between catalyst nanoparticles and supports presents a unique opportunity to enhance the stability, activity, and selectivity of heterogeneous catalysts. While charge transfer is tunable using the atomic structure and chemistry of the catalyst-support interface, direct experimental evidence is missing for three-dimensional catalyst nanoparticles, primarily due to the lack of a high-resolution method that can probe and correlate both the charge distribution and atomic structure of catalyst/support interfaces in these structures. We demonstrate a robust scanning transmission electron microscopy (STEM) method that simultaneously visualizes the atomic-scale structure and sub-nanometer-scale charge distribution in heterogeneous catalysts using a model Au-catalyst/SrTiO3-support system. Using this method, we further reveal the atomic-scale mechanisms responsible for the highly active perimeter sites and demonstrate that the charge transfer behavior can be readily controlled using post-synthesis treatments. This methodology provides a blueprint for better understanding the role of charge transfer in catalyst stability and performance and facilitates the future development of highly active advanced catalysts.

Date: 2022
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DOI: 10.1038/s41467-022-30923-2

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