Revealing the Phase Separation Behavior of Thermodynamically Immiscible Elements in a Nanoparticle
Abstract
Phase-separation is commonly observed in multimetallic nanomaterials, yet it is not well understood how immiscible elements distribute in a thermodynamically stable nanoparticle. Herein, we studied the phase-separation of Au and Rh in nanoparticles using electron microscopy and tomography techniques. The nanoparticles were thermally annealed to form thermodynamically stable structures. HAADF-STEM and EDS characterizations reveal that Au and Rh segregate into two domains while their miscibility is increased. Using aberration-corrected HAADF-STEM and atomic electron tomography, we show that the increased solubility of Au in Rh is achieved by forming Au clusters and single atoms inside the Rh domains and on the Rh surface. Furthermore, based on the three-dimensional reconstruction of a AuRh nanoparticle, we can visualize the uneven interface that is embedded in the nanoparticle. Finally, the results advance our understanding on the nanoscale thermodynamic behavior of metal mixtures, which is crucial for the optimization of multimetallic nanostructures for many applications.
- Authors:
-
[1];
[2];
[2];
[1];
[2];
[2]
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1821155
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 21; Journal Issue: 15; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; interfaces; metal nanoparticles; scanning transmission electron microscopy; gold; nanoparticles; heterostructured nanoparticle; phase separation; thermodynamics; electron tomography
Citation Formats
Chen, Peng-Cheng, Gao, Mengyu, Yu, Sunmoon, Jin, Jianbo, Song, Chengyu, Salmeron, Miquel, Scott, Mary C., and Yang, Peidong. Revealing the Phase Separation Behavior of Thermodynamically Immiscible Elements in a Nanoparticle. United States: N. p., 2021.
Web. doi:10.1021/acs.nanolett.1c02225.
Chen, Peng-Cheng, Gao, Mengyu, Yu, Sunmoon, Jin, Jianbo, Song, Chengyu, Salmeron, Miquel, Scott, Mary C., & Yang, Peidong. Revealing the Phase Separation Behavior of Thermodynamically Immiscible Elements in a Nanoparticle. United States. https://doi.org/10.1021/acs.nanolett.1c02225
Chen, Peng-Cheng, Gao, Mengyu, Yu, Sunmoon, Jin, Jianbo, Song, Chengyu, Salmeron, Miquel, Scott, Mary C., and Yang, Peidong. Tue .
"Revealing the Phase Separation Behavior of Thermodynamically Immiscible Elements in a Nanoparticle". United States. https://doi.org/10.1021/acs.nanolett.1c02225. https://www.osti.gov/servlets/purl/1821155.
@article{osti_1821155,
title = {Revealing the Phase Separation Behavior of Thermodynamically Immiscible Elements in a Nanoparticle},
author = {Chen, Peng-Cheng and Gao, Mengyu and Yu, Sunmoon and Jin, Jianbo and Song, Chengyu and Salmeron, Miquel and Scott, Mary C. and Yang, Peidong},
abstractNote = {Phase-separation is commonly observed in multimetallic nanomaterials, yet it is not well understood how immiscible elements distribute in a thermodynamically stable nanoparticle. Herein, we studied the phase-separation of Au and Rh in nanoparticles using electron microscopy and tomography techniques. The nanoparticles were thermally annealed to form thermodynamically stable structures. HAADF-STEM and EDS characterizations reveal that Au and Rh segregate into two domains while their miscibility is increased. Using aberration-corrected HAADF-STEM and atomic electron tomography, we show that the increased solubility of Au in Rh is achieved by forming Au clusters and single atoms inside the Rh domains and on the Rh surface. Furthermore, based on the three-dimensional reconstruction of a AuRh nanoparticle, we can visualize the uneven interface that is embedded in the nanoparticle. Finally, the results advance our understanding on the nanoscale thermodynamic behavior of metal mixtures, which is crucial for the optimization of multimetallic nanostructures for many applications.},
doi = {10.1021/acs.nanolett.1c02225},
journal = {Nano Letters},
number = 15,
volume = 21,
place = {United States},
year = {2021},
month = {7}
}
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