Tunable properties of PtxFe1-x electrocatalysts and their catalytic activity towards the oxygen reduction reaction

Feng Ju Lai, Hung Lung Chou, Loka Subramanyam Sarma, Di Yan Wang, Yen Chen Lin, Jyh Fu Lee, Bing Joe Hwang, Chia Chun Chen

Research output: Contribution to journalArticle

30 Citations (Scopus)

Abstract

We present the controlled synthesis of bimetallic PtxFe 1-x nanoparticles with tunable physical properties and a study of their catalytic activity towards the oxygen reduction reaction (ORR). Composition-induced variations in alloying extent and Pt d-band vacancies in Pt-Fe/C catalysts are systematically investigated. Density functional theoretical calculations are performed in order to realize the electronic effect caused by alloying Pt with Fe. The DFT computational observations revealed that iron donates electrons to platinum, when the Fe 3d and Pt 5d orbitals undergo hybridization. The PtxFe1-x catalysts with various Pt-to-Fe atomic ratios are characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), cyclic voltammetry (CV), and X-ray absorption spectroscopy (XAS). TEM images indicate that the dispersion of the metal nanoparticles is uniform and the XAS technique provides significant insight on Pt d-band vacancies and the alloying extent of Pt and Fe in Pt xFe1-x nanoparticles. Rotating-disk voltammetry of Pt xFe1-x nanoparticle catalysts with various Pt:Fe atomic compositions (3:1, 1:1, and 1:3) revealed that the Pt1Fe 1/C nanocatalyst showed a greater enhancement in ORR activity than platinum. The enhanced catalytic activity toward ORR is attributed to the higher alloying extent of platinum and iron as well as the promising electronic structure offered by the lower unfilled Pt d states in PtxFe 1-x nanoparticles when compared to pure Pt.

Original languageEnglish
Pages (from-to)573-581
Number of pages9
JournalNanoscale
Volume2
Issue number4
DOIs
Publication statusPublished - 2010 Apr 19

Fingerprint

Electrocatalysts
Alloying
Catalyst activity
Platinum
Oxygen
Nanoparticles
X ray absorption spectroscopy
Catalysts
Vacancies
Iron
Transmission electron microscopy
Metal nanoparticles
Rotating disks
Voltammetry
Chemical analysis
Discrete Fourier transforms
Cyclic voltammetry
Electronic structure
Density functional theory
Physical properties

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Tunable properties of PtxFe1-x electrocatalysts and their catalytic activity towards the oxygen reduction reaction. / Lai, Feng Ju; Chou, Hung Lung; Sarma, Loka Subramanyam; Wang, Di Yan; Lin, Yen Chen; Lee, Jyh Fu; Hwang, Bing Joe; Chen, Chia Chun.

In: Nanoscale, Vol. 2, No. 4, 19.04.2010, p. 573-581.

Research output: Contribution to journalArticle

Lai, Feng Ju ; Chou, Hung Lung ; Sarma, Loka Subramanyam ; Wang, Di Yan ; Lin, Yen Chen ; Lee, Jyh Fu ; Hwang, Bing Joe ; Chen, Chia Chun. / Tunable properties of PtxFe1-x electrocatalysts and their catalytic activity towards the oxygen reduction reaction. In: Nanoscale. 2010 ; Vol. 2, No. 4. pp. 573-581.
@article{684317a91a0a406ca9709dd8cd1881b8,
title = "Tunable properties of PtxFe1-x electrocatalysts and their catalytic activity towards the oxygen reduction reaction",
abstract = "We present the controlled synthesis of bimetallic PtxFe 1-x nanoparticles with tunable physical properties and a study of their catalytic activity towards the oxygen reduction reaction (ORR). Composition-induced variations in alloying extent and Pt d-band vacancies in Pt-Fe/C catalysts are systematically investigated. Density functional theoretical calculations are performed in order to realize the electronic effect caused by alloying Pt with Fe. The DFT computational observations revealed that iron donates electrons to platinum, when the Fe 3d and Pt 5d orbitals undergo hybridization. The PtxFe1-x catalysts with various Pt-to-Fe atomic ratios are characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), cyclic voltammetry (CV), and X-ray absorption spectroscopy (XAS). TEM images indicate that the dispersion of the metal nanoparticles is uniform and the XAS technique provides significant insight on Pt d-band vacancies and the alloying extent of Pt and Fe in Pt xFe1-x nanoparticles. Rotating-disk voltammetry of Pt xFe1-x nanoparticle catalysts with various Pt:Fe atomic compositions (3:1, 1:1, and 1:3) revealed that the Pt1Fe 1/C nanocatalyst showed a greater enhancement in ORR activity than platinum. The enhanced catalytic activity toward ORR is attributed to the higher alloying extent of platinum and iron as well as the promising electronic structure offered by the lower unfilled Pt d states in PtxFe 1-x nanoparticles when compared to pure Pt.",
author = "Lai, {Feng Ju} and Chou, {Hung Lung} and Sarma, {Loka Subramanyam} and Wang, {Di Yan} and Lin, {Yen Chen} and Lee, {Jyh Fu} and Hwang, {Bing Joe} and Chen, {Chia Chun}",
year = "2010",
month = "4",
day = "19",
doi = "10.1039/b9nr00239a",
language = "English",
volume = "2",
pages = "573--581",
journal = "Nanoscale",
issn = "2040-3364",
publisher = "Royal Society of Chemistry",
number = "4",

}

TY - JOUR

T1 - Tunable properties of PtxFe1-x electrocatalysts and their catalytic activity towards the oxygen reduction reaction

AU - Lai, Feng Ju

AU - Chou, Hung Lung

AU - Sarma, Loka Subramanyam

AU - Wang, Di Yan

AU - Lin, Yen Chen

AU - Lee, Jyh Fu

AU - Hwang, Bing Joe

AU - Chen, Chia Chun

PY - 2010/4/19

Y1 - 2010/4/19

N2 - We present the controlled synthesis of bimetallic PtxFe 1-x nanoparticles with tunable physical properties and a study of their catalytic activity towards the oxygen reduction reaction (ORR). Composition-induced variations in alloying extent and Pt d-band vacancies in Pt-Fe/C catalysts are systematically investigated. Density functional theoretical calculations are performed in order to realize the electronic effect caused by alloying Pt with Fe. The DFT computational observations revealed that iron donates electrons to platinum, when the Fe 3d and Pt 5d orbitals undergo hybridization. The PtxFe1-x catalysts with various Pt-to-Fe atomic ratios are characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), cyclic voltammetry (CV), and X-ray absorption spectroscopy (XAS). TEM images indicate that the dispersion of the metal nanoparticles is uniform and the XAS technique provides significant insight on Pt d-band vacancies and the alloying extent of Pt and Fe in Pt xFe1-x nanoparticles. Rotating-disk voltammetry of Pt xFe1-x nanoparticle catalysts with various Pt:Fe atomic compositions (3:1, 1:1, and 1:3) revealed that the Pt1Fe 1/C nanocatalyst showed a greater enhancement in ORR activity than platinum. The enhanced catalytic activity toward ORR is attributed to the higher alloying extent of platinum and iron as well as the promising electronic structure offered by the lower unfilled Pt d states in PtxFe 1-x nanoparticles when compared to pure Pt.

AB - We present the controlled synthesis of bimetallic PtxFe 1-x nanoparticles with tunable physical properties and a study of their catalytic activity towards the oxygen reduction reaction (ORR). Composition-induced variations in alloying extent and Pt d-band vacancies in Pt-Fe/C catalysts are systematically investigated. Density functional theoretical calculations are performed in order to realize the electronic effect caused by alloying Pt with Fe. The DFT computational observations revealed that iron donates electrons to platinum, when the Fe 3d and Pt 5d orbitals undergo hybridization. The PtxFe1-x catalysts with various Pt-to-Fe atomic ratios are characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), cyclic voltammetry (CV), and X-ray absorption spectroscopy (XAS). TEM images indicate that the dispersion of the metal nanoparticles is uniform and the XAS technique provides significant insight on Pt d-band vacancies and the alloying extent of Pt and Fe in Pt xFe1-x nanoparticles. Rotating-disk voltammetry of Pt xFe1-x nanoparticle catalysts with various Pt:Fe atomic compositions (3:1, 1:1, and 1:3) revealed that the Pt1Fe 1/C nanocatalyst showed a greater enhancement in ORR activity than platinum. The enhanced catalytic activity toward ORR is attributed to the higher alloying extent of platinum and iron as well as the promising electronic structure offered by the lower unfilled Pt d states in PtxFe 1-x nanoparticles when compared to pure Pt.

UR - http://www.scopus.com/inward/record.url?scp=77953680377&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=77953680377&partnerID=8YFLogxK

U2 - 10.1039/b9nr00239a

DO - 10.1039/b9nr00239a

M3 - Article

C2 - 20644761

AN - SCOPUS:77953680377

VL - 2

SP - 573

EP - 581

JO - Nanoscale

JF - Nanoscale

SN - 2040-3364

IS - 4

ER -