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Title: Dealloying in Individual Nanoparticles and Thin Film Grains: A Bragg Coherent Diffractive Imaging Study

Abstract

Dealloying is a process whereby selective dissolution results in a porous, strained structure often with new properties. The process is of both intrinsic and applied interest, and recently has been used to make highly active catalysts. The porosity has been studied using electron microscopy while the dealloying-induced strain has been studied at the ensemble level using X-ray diffraction. Despite the importance of local, for example, at the individual particle or grain level, strain in controlling the properties of the dealloyed material, it remains unresolved due to the difficulty of imaging 3D strain distributions with nanometer resolution in reactive environments. This information could play an integral role in understanding and controlling lattice strain for a variety of applications. Here, 3D strain distributions in individual nanoparticles and thin film grains in silver-gold alloys undergoing nitric acid-induced dealloying are imaged by Bragg coherent diffractive imaging. Particles exhibit dramatic changes in their local strains due to dealloying but grains do not. Furthermore, the average lattice in both grains and particles contracts during dealloying. In general, the results reveal significant dealloying-induced strain heterogeneity at the nanoscale in both isolated and extended samples, which may be utilized to develop advanced nanostructures for a variety of importantmore » applications.« less

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences and Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1372678
Alternate Identifier(s):
OSTI ID: 1401304
Grant/Contract Number:
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 25; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY

Citation Formats

Cha, Wonsuk, Liu, Yihua, You, Hoydoo, Stephenson, Gregory Brian, and Ulvestad, Andrew. Dealloying in Individual Nanoparticles and Thin Film Grains: A Bragg Coherent Diffractive Imaging Study. United States: N. p., 2017. Web. doi:10.1002/adfm.201700331.
Cha, Wonsuk, Liu, Yihua, You, Hoydoo, Stephenson, Gregory Brian, & Ulvestad, Andrew. Dealloying in Individual Nanoparticles and Thin Film Grains: A Bragg Coherent Diffractive Imaging Study. United States. doi:10.1002/adfm.201700331.
Cha, Wonsuk, Liu, Yihua, You, Hoydoo, Stephenson, Gregory Brian, and Ulvestad, Andrew. Tue . "Dealloying in Individual Nanoparticles and Thin Film Grains: A Bragg Coherent Diffractive Imaging Study". United States. doi:10.1002/adfm.201700331. https://www.osti.gov/servlets/purl/1372678.
@article{osti_1372678,
title = {Dealloying in Individual Nanoparticles and Thin Film Grains: A Bragg Coherent Diffractive Imaging Study},
author = {Cha, Wonsuk and Liu, Yihua and You, Hoydoo and Stephenson, Gregory Brian and Ulvestad, Andrew},
abstractNote = {Dealloying is a process whereby selective dissolution results in a porous, strained structure often with new properties. The process is of both intrinsic and applied interest, and recently has been used to make highly active catalysts. The porosity has been studied using electron microscopy while the dealloying-induced strain has been studied at the ensemble level using X-ray diffraction. Despite the importance of local, for example, at the individual particle or grain level, strain in controlling the properties of the dealloyed material, it remains unresolved due to the difficulty of imaging 3D strain distributions with nanometer resolution in reactive environments. This information could play an integral role in understanding and controlling lattice strain for a variety of applications. Here, 3D strain distributions in individual nanoparticles and thin film grains in silver-gold alloys undergoing nitric acid-induced dealloying are imaged by Bragg coherent diffractive imaging. Particles exhibit dramatic changes in their local strains due to dealloying but grains do not. Furthermore, the average lattice in both grains and particles contracts during dealloying. In general, the results reveal significant dealloying-induced strain heterogeneity at the nanoscale in both isolated and extended samples, which may be utilized to develop advanced nanostructures for a variety of important applications.},
doi = {10.1002/adfm.201700331},
journal = {Advanced Functional Materials},
number = 25,
volume = 27,
place = {United States},
year = {Tue May 09 00:00:00 EDT 2017},
month = {Tue May 09 00:00:00 EDT 2017}
}

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  • Cited by 2
  • Dissolution is critical to nanomaterial stability, especially for partially dealloyed nanoparticle catalysts. Unfortunately, highly active catalysts are often not stable in their reactive environments, preventing widespread application. Thus, focusing on the structure–stability relationship at the nanoscale is crucial and will likely play an important role in meeting grand challenges. Recent advances in imaging capability have come from electron, X-ray, and other techniques but tend to be limited to specific sample environments and/or two-dimensional images. Here, we report investigations into the defect-stability relationship of silver nanoparticles to voltage-induced electrochemical dissolution imaged in situ in three dimensional detail by Bragg coherent diffractivemore » imaging. We first determine the average dissolution kinetics by stationary probe rotating disk electrode in combination with inductively coupled plasma mass spectrometry, which allows in situ measurement of Ag+ ion formation. We then observe the dissolution and redeposition processes in single nanocrystals, providing unique insight about the role of surface strain, defects, and their coupling to the dissolution chemistry. Finally, the methods developed and the knowledge gained go well beyond a “simple” silver electrochemistry and are applicable to all electrocatalytic reactions where functional links between activity and stability are controlled by structure and defect dynamics.« less
  • Cited by 2
  • Here, we observed changes in morphology and internal strain state of commercial diamond nanocrystals during high-temperature annealing. Three nanodiamonds were measured with Bragg coherent x-ray diffraction imaging, yielding three-dimensional strain-sensitive images as a function of time/temperature. Up to temperatures of 800 °C, crystals with Gaussian strain distributions with a full-width-at-half-maximum of less than 8 × 10 –4 were largely unchanged, and annealing-induced strain relaxation was observed in a nanodiamond with maximum lattice distortions above this threshold. X-ray measurements found changes in nanodiamond morphology at temperatures above 600 °C that are consistent with graphitization of the surface, a result verified withmore » ensemble Raman measurements.« less