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

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. In conclusion, these results highlight the effect of particle shape and dimension on thermodynamics, informing nanorod design for improved device cyclability.

Authors:
 [1];  [1];  [2];  [3];  [1];  [2];  [1];  [4]
  1. Stanford Univ., Stanford, CA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. DIFFER - Dutch Institute for Fundamental Energy Research, Eindhoven (The Netherlands)
  4. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1458738
Grant/Contract Number:
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Hayee, Fariah, Narayan, Tarun C., Nadkarni, Neel, Baldi, Andrea, Koh, Ai Leen, Bazant, Martin Z., Sinclair, Robert, and Dionne, Jennifer A. In-situ visualization of solute-driven phase coexistence within individual nanorods. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04021-1.
Hayee, Fariah, Narayan, Tarun C., Nadkarni, Neel, Baldi, Andrea, Koh, Ai Leen, Bazant, Martin Z., Sinclair, Robert, & Dionne, Jennifer A. In-situ visualization of solute-driven phase coexistence within individual nanorods. United States. doi:10.1038/s41467-018-04021-1.
Hayee, Fariah, Narayan, Tarun C., Nadkarni, Neel, Baldi, Andrea, Koh, Ai Leen, Bazant, Martin Z., Sinclair, Robert, and Dionne, Jennifer A. Wed . "In-situ visualization of solute-driven phase coexistence within individual nanorods". United States. doi:10.1038/s41467-018-04021-1. https://www.osti.gov/servlets/purl/1458738.
@article{osti_1458738,
title = {In-situ visualization of solute-driven phase coexistence within individual nanorods},
author = {Hayee, Fariah and Narayan, Tarun C. and Nadkarni, Neel and Baldi, Andrea and Koh, Ai Leen and Bazant, Martin Z. and Sinclair, Robert and Dionne, Jennifer A.},
abstractNote = {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. In conclusion, these results highlight the effect of particle shape and dimension on thermodynamics, informing nanorod design for improved device cyclability.},
doi = {10.1038/s41467-018-04021-1},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Wed May 02 00:00:00 EDT 2018},
month = {Wed May 02 00:00:00 EDT 2018}
}

Journal Article:
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