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Title: Palladium-Coated Platinum Powders with Tunable, Nanostructured Surfaces for Applications in Catalysis

Abstract

Simultaneous control of nanoscale surface morphology and composition remains a challenge in preparing bimetallic catalysts, particularly at the large scale required for industrial application and with high-surface-area substrates. Atomic layer electroless deposition (ALED) is a scalable approach to prepare surface-modified metal powders in which elements more noble than the surface hydrides of the substrate metal are deposited layer-by-layer in a surface-limited fashion. In this paper, we demonstrate that high-surface-area Pt powder is a viable substrate for controlled deposition of Pd adlayers using this technique, with the potential for large-scale preparation, for use in electrocatalytic and catalytic applications such as fuel cells and functionalization of petrochemical feedstocks. Two different growth mechanisms have been proposed based on bulk and surface Pd atomic fractions obtained from atomic absorption spectroscopy and X-ray photoelectron spectroscopy, respectively. Further, spectral simulations were performed to strengthen the proposed growth mechanisms, favoring conformal growth in initial deposition followed by island formation in subsequent cycles. Observation of multiple pathways suggests a means of controlling adlayer surface morphology of ALED materials, in which an initial cycle of deposition sets the fractional coverage and subsequent cycles tune adlayer thickness.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Massachusetts, Dartmouth, MA (United States). Dept. of Chemistry and Biochemistry
  2. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); US Army Research Laboratory (USARL)
OSTI Identifier:
1634805
Report Number(s):
SAND-2020-5696J
Journal ID: ISSN 2574-0970; 686459
Grant/Contract Number:  
AC04-94AL85000; NA0003525; 1726239; W911NF-16-1-0438
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Nano Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2574-0970
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ALD; ALED; electroless; surface alloy; growth mechanism; galvanic replacement; surface hydride; surface-limited redox replacment (SLRR); near-surface alloy

Citation Formats

Gurung, Sita, Robinson, David B., and Cappillino, Patrick J.. Palladium-Coated Platinum Powders with Tunable, Nanostructured Surfaces for Applications in Catalysis. United States: N. p., 2019. Web. https://doi.org/10.1021/acsanm.9b02090.
Gurung, Sita, Robinson, David B., & Cappillino, Patrick J.. Palladium-Coated Platinum Powders with Tunable, Nanostructured Surfaces for Applications in Catalysis. United States. https://doi.org/10.1021/acsanm.9b02090
Gurung, Sita, Robinson, David B., and Cappillino, Patrick J.. Fri . "Palladium-Coated Platinum Powders with Tunable, Nanostructured Surfaces for Applications in Catalysis". United States. https://doi.org/10.1021/acsanm.9b02090. https://www.osti.gov/servlets/purl/1634805.
@article{osti_1634805,
title = {Palladium-Coated Platinum Powders with Tunable, Nanostructured Surfaces for Applications in Catalysis},
author = {Gurung, Sita and Robinson, David B. and Cappillino, Patrick J.},
abstractNote = {Simultaneous control of nanoscale surface morphology and composition remains a challenge in preparing bimetallic catalysts, particularly at the large scale required for industrial application and with high-surface-area substrates. Atomic layer electroless deposition (ALED) is a scalable approach to prepare surface-modified metal powders in which elements more noble than the surface hydrides of the substrate metal are deposited layer-by-layer in a surface-limited fashion. In this paper, we demonstrate that high-surface-area Pt powder is a viable substrate for controlled deposition of Pd adlayers using this technique, with the potential for large-scale preparation, for use in electrocatalytic and catalytic applications such as fuel cells and functionalization of petrochemical feedstocks. Two different growth mechanisms have been proposed based on bulk and surface Pd atomic fractions obtained from atomic absorption spectroscopy and X-ray photoelectron spectroscopy, respectively. Further, spectral simulations were performed to strengthen the proposed growth mechanisms, favoring conformal growth in initial deposition followed by island formation in subsequent cycles. Observation of multiple pathways suggests a means of controlling adlayer surface morphology of ALED materials, in which an initial cycle of deposition sets the fractional coverage and subsequent cycles tune adlayer thickness.},
doi = {10.1021/acsanm.9b02090},
journal = {ACS Applied Nano Materials},
number = 1,
volume = 3,
place = {United States},
year = {2019},
month = {12}
}

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