Oleylamine aging of ptni nanoparticles giving enhanced functionality for the oxygen reduction reaction

Gerard M. Leteba; Yi-Chi Wang; Thomas J. A. Slater; Rongsheng Cai; Conor Byrne; Christopher P. Race; David R. G. Mitchell; Pieter B. J. Levecque; Neil P. Young; Stuart M. Holmes; Alex Walton; Angus I. Kirkland; Sarah J. Haigh; Candace I. Lang

doi:10.1021/acs.nanolett.1c00706

Oleylamine aging of ptni nanoparticles giving enhanced functionality for the oxygen reduction reaction

Gerard M. Leteba, Yi-Chi Wang, Thomas J. A. Slater, Rongsheng Cai, Conor Byrne, Christopher P. Race, David R. G. Mitchell, Pieter B. J. Levecque, Neil P. Young, Stuart M. Holmes, Alex Walton, Angus I. Kirkland, Sarah J. Haigh^*, Candace I. Lang^*

^*Corresponding author for this work

School of Engineering

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

54 Citations (Scopus)

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Abstract

[Graphic presents]

We report a rapid solution-phase strategy to synthesize alloyed PtNi nanoparticles which demonstrate outstanding functionality for the oxygen reduction reaction (ORR). This one-pot coreduction colloidal synthesis results in a monodisperse population of single-crystal nanoparticles of rhombic dodecahedral morphology with Pt-enriched edges and compositions close to Pt₁Ni₂. We use nanoscale 3D compositional analysis to reveal for the first time that oleylamine (OAm)-aging of the rhombic dodecahedral Pt₁Ni₂ particles results in Ni leaching from surface facets, producing aged particles with concave faceting, an exceptionally high surface area, and a composition of Pt₂Ni₁. We show that the modified atomic nanostructures catalytically outperform the original PtNi rhombic dodecahedral particles by more than two-fold and also yield improved cycling durability. Their functionality for the ORR far exceeds commercially available Pt/C nanoparticle electrocatalysts, both in terms of mass-specific activities (up to a 25-fold increase) and intrinsic area-specific activities (up to a 27-fold increase).

Original language	English
Pages (from-to)	3989–3996
Number of pages	8
Journal	Nano Letters
Volume	21
Issue number	9
DOIs	https://doi.org/10.1021/acs.nanolett.1c00706
Publication status	Published - 12 May 2021

Bibliographical note

Copyright the Author(s) 2021. Version archived for private and non-commercial use with the permission of the author/s and according to publisher conditions. For further rights please contact the publisher.

Keywords

ORR
electrocatalyst
nanoparticle
electron tomography
STEM-EDS
PEMFC

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10.1021/acs.nanolett.1c00706Licence: CC BY

Publisher version (open access)Final published version, 707 KBLicence: CC BY

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Leteba, G. M., Wang, Y.-C., Slater, T. J. A., Cai, R., Byrne, C., Race, C. P., Mitchell, D. R. G., Levecque, P. B. J., Young, N. P., Holmes, S. M., Walton, A., Kirkland, A. I., Haigh, S. J., & Lang, C. I. (2021). Oleylamine aging of ptni nanoparticles giving enhanced functionality for the oxygen reduction reaction. Nano Letters, 21(9), 3989–3996. https://doi.org/10.1021/acs.nanolett.1c00706

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title = "Oleylamine aging of ptni nanoparticles giving enhanced functionality for the oxygen reduction reaction",

abstract = "[Graphic presents] We report a rapid solution-phase strategy to synthesize alloyed PtNi nanoparticles which demonstrate outstanding functionality for the oxygen reduction reaction (ORR). This one-pot coreduction colloidal synthesis results in a monodisperse population of single-crystal nanoparticles of rhombic dodecahedral morphology with Pt-enriched edges and compositions close to Pt1Ni2. We use nanoscale 3D compositional analysis to reveal for the first time that oleylamine (OAm)-aging of the rhombic dodecahedral Pt1Ni2 particles results in Ni leaching from surface facets, producing aged particles with concave faceting, an exceptionally high surface area, and a composition of Pt2Ni1. We show that the modified atomic nanostructures catalytically outperform the original PtNi rhombic dodecahedral particles by more than two-fold and also yield improved cycling durability. Their functionality for the ORR far exceeds commercially available Pt/C nanoparticle electrocatalysts, both in terms of mass-specific activities (up to a 25-fold increase) and intrinsic area-specific activities (up to a 27-fold increase).",

keywords = "ORR, electrocatalyst, nanoparticle, electron tomography, STEM-EDS, PEMFC",

author = "Leteba, \{Gerard M.\} and Yi-Chi Wang and Slater, \{Thomas J. A.\} and Rongsheng Cai and Conor Byrne and Race, \{Christopher P.\} and Mitchell, \{David R. G.\} and Levecque, \{Pieter B. J.\} and Young, \{Neil P.\} and Holmes, \{Stuart M.\} and Alex Walton and Kirkland, \{Angus I.\} and Haigh, \{Sarah J.\} and Lang, \{Candace I.\}",

note = "Copyright the Author(s) 2021. Version archived for private and non-commercial use with the permission of the author/s and according to publisher conditions. For further rights please contact the publisher.",

year = "2021",

month = may,

day = "12",

doi = "10.1021/acs.nanolett.1c00706",

language = "English",

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T1 - Oleylamine aging of ptni nanoparticles giving enhanced functionality for the oxygen reduction reaction

AU - Leteba, Gerard M.

AU - Wang, Yi-Chi

AU - Slater, Thomas J. A.

AU - Cai, Rongsheng

AU - Byrne, Conor

AU - Race, Christopher P.

AU - Mitchell, David R. G.

AU - Levecque, Pieter B. J.

AU - Young, Neil P.

AU - Holmes, Stuart M.

AU - Walton, Alex

AU - Kirkland, Angus I.

AU - Haigh, Sarah J.

AU - Lang, Candace I.

N1 - Copyright the Author(s) 2021. Version archived for private and non-commercial use with the permission of the author/s and according to publisher conditions. For further rights please contact the publisher.

PY - 2021/5/12

Y1 - 2021/5/12

N2 - [Graphic presents] We report a rapid solution-phase strategy to synthesize alloyed PtNi nanoparticles which demonstrate outstanding functionality for the oxygen reduction reaction (ORR). This one-pot coreduction colloidal synthesis results in a monodisperse population of single-crystal nanoparticles of rhombic dodecahedral morphology with Pt-enriched edges and compositions close to Pt1Ni2. We use nanoscale 3D compositional analysis to reveal for the first time that oleylamine (OAm)-aging of the rhombic dodecahedral Pt1Ni2 particles results in Ni leaching from surface facets, producing aged particles with concave faceting, an exceptionally high surface area, and a composition of Pt2Ni1. We show that the modified atomic nanostructures catalytically outperform the original PtNi rhombic dodecahedral particles by more than two-fold and also yield improved cycling durability. Their functionality for the ORR far exceeds commercially available Pt/C nanoparticle electrocatalysts, both in terms of mass-specific activities (up to a 25-fold increase) and intrinsic area-specific activities (up to a 27-fold increase).

AB - [Graphic presents] We report a rapid solution-phase strategy to synthesize alloyed PtNi nanoparticles which demonstrate outstanding functionality for the oxygen reduction reaction (ORR). This one-pot coreduction colloidal synthesis results in a monodisperse population of single-crystal nanoparticles of rhombic dodecahedral morphology with Pt-enriched edges and compositions close to Pt1Ni2. We use nanoscale 3D compositional analysis to reveal for the first time that oleylamine (OAm)-aging of the rhombic dodecahedral Pt1Ni2 particles results in Ni leaching from surface facets, producing aged particles with concave faceting, an exceptionally high surface area, and a composition of Pt2Ni1. We show that the modified atomic nanostructures catalytically outperform the original PtNi rhombic dodecahedral particles by more than two-fold and also yield improved cycling durability. Their functionality for the ORR far exceeds commercially available Pt/C nanoparticle electrocatalysts, both in terms of mass-specific activities (up to a 25-fold increase) and intrinsic area-specific activities (up to a 27-fold increase).

KW - ORR

KW - electrocatalyst

KW - nanoparticle

KW - electron tomography

KW - STEM-EDS

KW - PEMFC

UR - https://www.scopus.com/pages/publications/85105967454

UR - http://purl.org/au-research/grants/arc/LE120100104

U2 - 10.1021/acs.nanolett.1c00706

DO - 10.1021/acs.nanolett.1c00706

M3 - Article

C2 - 33899489

AN - SCOPUS:85105967454

SN - 1530-6984

VL - 21

SP - 3989

EP - 3996

JO - Nano Letters

JF - Nano Letters

IS - 9

ER -

Oleylamine aging of ptni nanoparticles giving enhanced functionality for the oxygen reduction reaction

Abstract

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