In-situ visualization of solute-driven phase coexistence within individual nanorods

Fariah Hayee; Tarun C. Narayan; Neel Nadkarni; Andrea Baldi; Ai Leen Koh; Martin Z. Bazant; Robert Sinclair; Jennifer A. Dionne

doi:10.1038/s41467-018-04021-1

In-situ visualization of solute-driven phase coexistence within individual nanorods

Fariah Hayee
, Tarun C. Narayan
, Neel Nadkarni
, Andrea Baldi
, Ai Leen Koh
, Martin Z. Bazant
, Robert Sinclair
, Jennifer A. Dionne

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Abstract

Nanorods are promising components of energy and information storage devices that rely on solute-driven phase transformations, due to their large surface-To-volume ratio and ability to accommodate strain. Here we investigate the hydrogen-induced phase transition in individual penta-Twinned palladium nanorods of varying aspect ratios with ~3 nm spatial resolution to understand the correlation between nanorod structure and thermodynamics. We find that the hydrogenated phase preferentially nucleates at the rod tips, progressing along the length of the nanorods with increasing hydrogen pressure. While nucleation pressure is nearly constant for all lengths, the number of phase boundaries is length-dependent, with stable phase coexistence always occurring for rods longer than 55 nm. Moreover, such coexistence occurs within individual crystallites of the nanorods and is accompanied by defect formation, as supported by in situ electron microscopy and elastic energy calculations. These results highlight the effect of particle shape and dimension on thermodynamics, informing nanorod design for improved device cyclability.

Original language	English
Article number	1775
Journal	Nature Communications
Volume	9
Issue number	1
DOIs	https://doi.org/10.1038/s41467-018-04021-1
Publication status	Published - 2 May 2018

Funding

We gratefully acknowledge scientific feedback from Dr. Ann F. Marshall and Ms. Katherine Sytwu. TEM imaging and spectroscopy were performed at the Stanford Nano Shared Facilities (SNSF). Support from a PECASE Award administered by the Air Force Office of Scientific Research (FA9550-15-1-0006), a National Science Foundation CAREER Award (DMR-1151231), a Camille and Henry Dreyfus grant are gratefully acknowledged. F.H. also acknowledges the support of SOE John Linvill Fellowship. A.B. acknowledges support from the research program fellowships for Young Energy Scientists’ (YES!) of the Foundation for Fundamental Research on Matter (FOM), which is financially supported by the Netherlands Organization for Scientific Research (NWO). T.C.N. was supported by an award from the Department of Energy (DOE) Office of Science Graduate Fellowship Program administered by the Oak Ridge Institute for Science and Education for the DOE. ORISE is managed by Oak Ridge Associated Universities (ORAU) under DOE contract number DE-AC05-06OR23100. M.Z.B. acknowledges the sabbatical leave at Stanford University supported by the Global Climate and Energy Project, and by the US Department of Energy, Basic Energy Sciences through the SUNCAT Center for Interface Science and Catalysis. All opinions expressed in this paper are the authors’ and do not necessarily reflect the policies and views of DOE, ORAU, or ORISE. ORISE is managed by Oak Ridge Associated Universities (ORAU) under DOE contract number DE-AC05-06OR23100

Funders	Funder number
Stichting voor Fundamenteel Onderzoek der Materie
Basic Energy Sciences
Oak Ridge Institute for Science and Education
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
Camille and Henry Dreyfus Foundation
Office of Science
Oak Ridge Associated Universities	DE-AC05-06OR23100
Air Force Office of Scientific Research	FA9550-15-1-0006
National Science Foundation	DMR-1151231
U.S. Department of Energy	DE-AC05-06OR23100

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

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10.1038/s41467-018-04021-1

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AU - Bazant, Martin Z.

AU - Sinclair, Robert

AU - Dionne, Jennifer A.

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In-situ visualization of solute-driven phase coexistence within individual nanorods

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