Phase-Controlled Synthesis of Ru Nanocrystals via Template-Directed Growth: Surface Energy versus Bulk Energy

Annemieke Janssen; Zhiheng Lyu; Marc Figueras-Valls; Hsin Yun Chao; Yifeng Shi; Veronica Pawlik; Miaofang Chi; Manos Mavrikakis; Younan Xia

doi:10.1021/acs.nanolett.1c05009

Phase-Controlled Synthesis of Ru Nanocrystals via Template-Directed Growth: Surface Energy versus Bulk Energy

Annemieke Janssen, Zhiheng Lyu, Marc Figueras-Valls, Hsin Yun Chao, Yifeng Shi, Veronica Pawlik, Miaofang Chi, Manos Mavrikakis, Younan Xia

electron Microscopy and Microanalysis

Research output: Contribution to journal › Article › peer-review

12 Scopus citations

Abstract

Despite the successful control of crystal phase using template-directed growth, much remains unknown about the underlying mechanisms. Here, we demonstrate that the crystal phase taken by the deposited metal depends on the lateral size of face-centered cubic (fcc)-Pd nanoplate templates with 12 nm plates giving fcc-Ru while 18-26 nm plates result in hexagonal closed-packed (hcp)-Ru. Although Ru overlayers with a metastable fcc- (high in bulk energy) or stable hcp-phase (low in bulk energy) can be epitaxially deposited on the basal planes, the lattice mismatch will lead to jagged hcp- (high in surface energy) and smooth fcc-facets (low in surface energy), respectively, on the side faces. As the proportion of basal and side faces on the nanoplates varies with lateral size, the crystal phase will change depending on the relative contributions from the surface and bulk energies. The Pd@fcc-Ru outperforms the Pd@hcp-Ru nanoplates toward ethylene glycol and glycerol oxidation reactions.

Original language	English
Pages (from-to)	3591-3597
Number of pages	7
Journal	Nano Letters
Volume	22
Issue number	9
DOIs	https://doi.org/10.1021/acs.nanolett.1c05009
State	Published - May 11 2022

Funding

This work was supported in part by a grant from the NSF (CHE 2105602) and start-up funds from the Georgia Institute of Technology. This work was performed in part at the Georgia Tech Institute for Electronics and Nanotechnology, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which is supported by the National Science Foundation (ECCS-2025462). H.C. and M.C. were supported by the U.S. Department of Energy (DOE), Office of Sciences, under early career Award No. ERKCZ55. Microscopy research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a U.S. DOE, Office of Science User Facility at Oak Ridge National Laboratory.

Funders	Funder number
Center for Nanophase Materials Sciences
National Science Foundation	ECCS-2025462, CHE 2105602
National Science Foundation
U.S. Department of Energy
Office of Science	ERKCZ55
Office of Science
Oak Ridge National Laboratory
Georgia Institute of Technology

Keywords

crystal phase
metal nanocrystal
metastable phase
polymorphism
structure−property relationship

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10.1021/acs.nanolett.1c05009

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title = "Phase-Controlled Synthesis of Ru Nanocrystals via Template-Directed Growth: Surface Energy versus Bulk Energy",

abstract = "Despite the successful control of crystal phase using template-directed growth, much remains unknown about the underlying mechanisms. Here, we demonstrate that the crystal phase taken by the deposited metal depends on the lateral size of face-centered cubic (fcc)-Pd nanoplate templates with 12 nm plates giving fcc-Ru while 18-26 nm plates result in hexagonal closed-packed (hcp)-Ru. Although Ru overlayers with a metastable fcc- (high in bulk energy) or stable hcp-phase (low in bulk energy) can be epitaxially deposited on the basal planes, the lattice mismatch will lead to jagged hcp- (high in surface energy) and smooth fcc-facets (low in surface energy), respectively, on the side faces. As the proportion of basal and side faces on the nanoplates varies with lateral size, the crystal phase will change depending on the relative contributions from the surface and bulk energies. The Pd@fcc-Ru outperforms the Pd@hcp-Ru nanoplates toward ethylene glycol and glycerol oxidation reactions.",

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AU - Chao, Hsin Yun

AU - Shi, Yifeng

AU - Pawlik, Veronica

AU - Chi, Miaofang

AU - Mavrikakis, Manos

AU - Xia, Younan

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N2 - Despite the successful control of crystal phase using template-directed growth, much remains unknown about the underlying mechanisms. Here, we demonstrate that the crystal phase taken by the deposited metal depends on the lateral size of face-centered cubic (fcc)-Pd nanoplate templates with 12 nm plates giving fcc-Ru while 18-26 nm plates result in hexagonal closed-packed (hcp)-Ru. Although Ru overlayers with a metastable fcc- (high in bulk energy) or stable hcp-phase (low in bulk energy) can be epitaxially deposited on the basal planes, the lattice mismatch will lead to jagged hcp- (high in surface energy) and smooth fcc-facets (low in surface energy), respectively, on the side faces. As the proportion of basal and side faces on the nanoplates varies with lateral size, the crystal phase will change depending on the relative contributions from the surface and bulk energies. The Pd@fcc-Ru outperforms the Pd@hcp-Ru nanoplates toward ethylene glycol and glycerol oxidation reactions.

AB - Despite the successful control of crystal phase using template-directed growth, much remains unknown about the underlying mechanisms. Here, we demonstrate that the crystal phase taken by the deposited metal depends on the lateral size of face-centered cubic (fcc)-Pd nanoplate templates with 12 nm plates giving fcc-Ru while 18-26 nm plates result in hexagonal closed-packed (hcp)-Ru. Although Ru overlayers with a metastable fcc- (high in bulk energy) or stable hcp-phase (low in bulk energy) can be epitaxially deposited on the basal planes, the lattice mismatch will lead to jagged hcp- (high in surface energy) and smooth fcc-facets (low in surface energy), respectively, on the side faces. As the proportion of basal and side faces on the nanoplates varies with lateral size, the crystal phase will change depending on the relative contributions from the surface and bulk energies. The Pd@fcc-Ru outperforms the Pd@hcp-Ru nanoplates toward ethylene glycol and glycerol oxidation reactions.

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Phase-Controlled Synthesis of Ru Nanocrystals via Template-Directed Growth: Surface Energy versus Bulk Energy

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