Core-Shell Nanostructured Au@NimPt2 Electrocatalysts with Enhanced Activity and Durability for Oxygen Reduction Reaction

Liu Liu Shen, Gui Rong Zhang, Shu Miao, Jingyue Liu, Bo Qing Xu

Research output: Contribution to journalArticle

35 Citations (Scopus)

Abstract

Fabricating Pt-alloy and core-shell nanostructures with Au NPs in the cores are considered as two general approaches to improving the performance of Pt-based catalysts for the cathodic oxygen reduction reaction (ORR) in acidic electrolyte. These two approaches are combined herein to develop a heteroseed-mediated solvothermal method for synthesizing nearly monodisperse core-shell structured Au@NimPt2 nanoparticles (NPs) of 5.0-6.5 nm (with the atomic ratio of Ni/Pt/Au = m/2/1) as ORR catalysts. With respect to controlling the amount and relative concentrations of the metal precursors in the starting solution, this method enables not only facile manipulation of the shell composition and thickness but also fine-tuning of the core-shell interaction and surface electronic structures of the resultant Au@NimPt2 NPs, endowing the Au@NimPt2 NPs with improved Pt activity and durability for ORR. Subjecting the Au@NimPt2 NPs to an ex situ pretreatment in flowing 2%CO/Ar at 300 °C is shown to result in further improved Pt activity. Data are also presented to correlate the intrinsic Pt activity with experimentally determined CO adsorption property (CO-stripping peak potential) of Pt for the Au@NimPt2 samples, and to show the excellent electrochemical durability of the Au@NimPt2 NPs during 20 000 potential cycles between 0.6 and 1.1 V (vs RHE) in O2-saturated 0.1 M HClO4. Compared with the commercial E-TEK Pt/C catalyst, the most-active Au@Ni2Pt2 NPs exhibit 3-4- and 4-6-fold higher Pt activity at 0.9 V before and after the 20 000 potential cycles, respectively. Factors relevant to the activity and durability control of the Au@NimPt2 catalysts for ORR are discussed.

Original languageEnglish (US)
Pages (from-to)1680-1690
Number of pages11
JournalACS Catalysis
Volume6
Issue number3
DOIs
StatePublished - Mar 4 2016

Fingerprint

Electrocatalysts
Durability
Oxygen
Nanoparticles
Carbon Monoxide
Catalysts
Shells (structures)
Electrolytes
Electronic structure
Nanostructures
Tuning
Metals
Adsorption
Chemical analysis

Keywords

  • catalyst design
  • core-shell nanostructure
  • electrocatalyst
  • electrochemical treatment
  • multimetallic nanoparticles
  • oxygen reduction reaction
  • solvothermal synthesis

ASJC Scopus subject areas

  • Catalysis

Cite this

Core-Shell Nanostructured Au@NimPt2 Electrocatalysts with Enhanced Activity and Durability for Oxygen Reduction Reaction. / Shen, Liu Liu; Zhang, Gui Rong; Miao, Shu; Liu, Jingyue; Xu, Bo Qing.

In: ACS Catalysis, Vol. 6, No. 3, 04.03.2016, p. 1680-1690.

Research output: Contribution to journalArticle

Shen, Liu Liu ; Zhang, Gui Rong ; Miao, Shu ; Liu, Jingyue ; Xu, Bo Qing. / Core-Shell Nanostructured Au@NimPt2 Electrocatalysts with Enhanced Activity and Durability for Oxygen Reduction Reaction. In: ACS Catalysis. 2016 ; Vol. 6, No. 3. pp. 1680-1690.
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abstract = "Fabricating Pt-alloy and core-shell nanostructures with Au NPs in the cores are considered as two general approaches to improving the performance of Pt-based catalysts for the cathodic oxygen reduction reaction (ORR) in acidic electrolyte. These two approaches are combined herein to develop a heteroseed-mediated solvothermal method for synthesizing nearly monodisperse core-shell structured Au@NimPt2 nanoparticles (NPs) of 5.0-6.5 nm (with the atomic ratio of Ni/Pt/Au = m/2/1) as ORR catalysts. With respect to controlling the amount and relative concentrations of the metal precursors in the starting solution, this method enables not only facile manipulation of the shell composition and thickness but also fine-tuning of the core-shell interaction and surface electronic structures of the resultant Au@NimPt2 NPs, endowing the Au@NimPt2 NPs with improved Pt activity and durability for ORR. Subjecting the Au@NimPt2 NPs to an ex situ pretreatment in flowing 2{\%}CO/Ar at 300 °C is shown to result in further improved Pt activity. Data are also presented to correlate the intrinsic Pt activity with experimentally determined CO adsorption property (CO-stripping peak potential) of Pt for the Au@NimPt2 samples, and to show the excellent electrochemical durability of the Au@NimPt2 NPs during 20{\^a}€¯000 potential cycles between 0.6 and 1.1 V (vs RHE) in O2-saturated 0.1 M HClO4. Compared with the commercial E-TEK Pt/C catalyst, the most-active Au@Ni2Pt2 NPs exhibit 3-4- and 4-6-fold higher Pt activity at 0.9 V before and after the 20{\^a}€¯000 potential cycles, respectively. Factors relevant to the activity and durability control of the Au@NimPt2 catalysts for ORR are discussed.",
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T1 - Core-Shell Nanostructured Au@NimPt2 Electrocatalysts with Enhanced Activity and Durability for Oxygen Reduction Reaction

AU - Shen, Liu Liu

AU - Zhang, Gui Rong

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AU - Liu, Jingyue

AU - Xu, Bo Qing

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N2 - Fabricating Pt-alloy and core-shell nanostructures with Au NPs in the cores are considered as two general approaches to improving the performance of Pt-based catalysts for the cathodic oxygen reduction reaction (ORR) in acidic electrolyte. These two approaches are combined herein to develop a heteroseed-mediated solvothermal method for synthesizing nearly monodisperse core-shell structured Au@NimPt2 nanoparticles (NPs) of 5.0-6.5 nm (with the atomic ratio of Ni/Pt/Au = m/2/1) as ORR catalysts. With respect to controlling the amount and relative concentrations of the metal precursors in the starting solution, this method enables not only facile manipulation of the shell composition and thickness but also fine-tuning of the core-shell interaction and surface electronic structures of the resultant Au@NimPt2 NPs, endowing the Au@NimPt2 NPs with improved Pt activity and durability for ORR. Subjecting the Au@NimPt2 NPs to an ex situ pretreatment in flowing 2%CO/Ar at 300 °C is shown to result in further improved Pt activity. Data are also presented to correlate the intrinsic Pt activity with experimentally determined CO adsorption property (CO-stripping peak potential) of Pt for the Au@NimPt2 samples, and to show the excellent electrochemical durability of the Au@NimPt2 NPs during 20 000 potential cycles between 0.6 and 1.1 V (vs RHE) in O2-saturated 0.1 M HClO4. Compared with the commercial E-TEK Pt/C catalyst, the most-active Au@Ni2Pt2 NPs exhibit 3-4- and 4-6-fold higher Pt activity at 0.9 V before and after the 20 000 potential cycles, respectively. Factors relevant to the activity and durability control of the Au@NimPt2 catalysts for ORR are discussed.

AB - Fabricating Pt-alloy and core-shell nanostructures with Au NPs in the cores are considered as two general approaches to improving the performance of Pt-based catalysts for the cathodic oxygen reduction reaction (ORR) in acidic electrolyte. These two approaches are combined herein to develop a heteroseed-mediated solvothermal method for synthesizing nearly monodisperse core-shell structured Au@NimPt2 nanoparticles (NPs) of 5.0-6.5 nm (with the atomic ratio of Ni/Pt/Au = m/2/1) as ORR catalysts. With respect to controlling the amount and relative concentrations of the metal precursors in the starting solution, this method enables not only facile manipulation of the shell composition and thickness but also fine-tuning of the core-shell interaction and surface electronic structures of the resultant Au@NimPt2 NPs, endowing the Au@NimPt2 NPs with improved Pt activity and durability for ORR. Subjecting the Au@NimPt2 NPs to an ex situ pretreatment in flowing 2%CO/Ar at 300 °C is shown to result in further improved Pt activity. Data are also presented to correlate the intrinsic Pt activity with experimentally determined CO adsorption property (CO-stripping peak potential) of Pt for the Au@NimPt2 samples, and to show the excellent electrochemical durability of the Au@NimPt2 NPs during 20 000 potential cycles between 0.6 and 1.1 V (vs RHE) in O2-saturated 0.1 M HClO4. Compared with the commercial E-TEK Pt/C catalyst, the most-active Au@Ni2Pt2 NPs exhibit 3-4- and 4-6-fold higher Pt activity at 0.9 V before and after the 20 000 potential cycles, respectively. Factors relevant to the activity and durability control of the Au@NimPt2 catalysts for ORR are discussed.

KW - catalyst design

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KW - electrochemical treatment

KW - multimetallic nanoparticles

KW - oxygen reduction reaction

KW - solvothermal synthesis

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