Imaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells

Lei Chen, Alberto Leonardi, Jun Chen, Muhan Cao, Na Li, Dong Su, Qiao Zhang (), Michael Engel () and Xingchen Ye ()
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Lei Chen: Soochow University
Alberto Leonardi: IZNF, Friedrich-Alexander University Erlangen-Nürnberg
Jun Chen: Indiana University
Muhan Cao: Indiana University
Na Li: Brookhaven National Laboratory
Dong Su: Brookhaven National Laboratory
Qiao Zhang: Soochow University
Michael Engel: IZNF, Friedrich-Alexander University Erlangen-Nürnberg
Xingchen Ye: Indiana University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Chemical design of multicomponent nanocrystals requires atomic-level understanding of reaction kinetics. Here, we apply single-particle imaging coupled with atomistic simulation to study reaction pathways and rates of Pd@Au and Cu@Au core-shell nanocubes undergoing oxidative dissolution. Quantitative analysis of etching kinetics using in situ transmission electron microscopy (TEM) imaging reveals that the dissolution mechanism changes from predominantly edge-selective to layer-by-layer removal of Au atoms as the reaction progresses. Dissolution of the Au shell slows down when both metals are exposed, which we attribute to galvanic corrosion protection. Morphological transformations are determined by intrinsic anisotropy due to coordination-number-dependent atom removal rates and extrinsic anisotropy induced by the graphene window. Our work demonstrates that bimetallic core-shell nanocrystals are excellent probes for the local physicochemical conditions inside TEM liquid cells. Furthermore, single-particle TEM imaging and atomistic simulation of reaction trajectories can inform future design strategies for compositionally and architecturally sophisticated nanocrystals.

Date: 2020
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DOI: 10.1038/s41467-020-16645-3

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