期刊
NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-16645-3
关键词
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资金
- Indiana University
- U.S. DOE Office of Science Facility at Brookhaven National Laboratory [DE-SC0012704]
- China Scholarship Council
- Deutscht Foschungsgemeinschaft through the Cluster of Excellence Engineering of Advanced Materials [EXC 315/2]
- Central Institute for Scientific Computing (ZISC)
- Interdisciplinary Center for Functional Particle Systems (FPS) at Friedrich-Alexander University Erlangen-Numberg
- Erlangen Regional Computing Center (RRZE)
- US DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
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.
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