Molybdenum-doped PdPt@Pt core−shell octahedra supported by ionic block copolymer-functionalized graphene as a highly active and durable oxygen reduction electrocatalyst

Kie Yong Cho, Yong Sik Yeom, Heun Young Seo, Pradip Kumar, Albert S. Lee, Kyung Youl Baek, Ho Gyu Yoon

Research output: Contribution to journalArticle

28 Citations (Scopus)

Abstract

Development of highly active and durable electrocatalysts that can effectively electrocatalyze oxygen reduction reactions (ORR) still remains one important challenge for high-performance electrochemical conversion and storage applications such as fuel cells and metal-air batteries. Herein, we propose the combination of molybdenum-doped PdPt@Pt core−shell octahedra and the pyrene-functionalized poly(dimethylaminoethyl methacrylate)-b-poly[(ethylene glycol) methyl ether methacrylate] ionic block copolymer-functionalized reduced graphene oxide (Mo-PdPt@Pt/IG) to effectively augment the interfacial cohesion of both components using a tunable ex situ mixing strategy. The rationally designed Mo-PdPt@Pt core−shell octahedra have unique compositional benefits, including segregation of Mo atoms on the vertexes and edges of the octahedron and 2−3 shell layers of Pt atoms on a PdPt alloy core, which can provide highly active sites to the catalyst for ORR along with enhanced electrochemical stability. In addition, the ionic block copolymer functionalized graphene can facilitate intermolecular charge transfer and good stability of metal NPs, which arises from the ionic block copolymer interfacial layer. When the beneficial features of the Mo-PdPt@Pt and IG are combined, the Mo-PdPt@Pt/IG exhibits substantially enhanced activity and durability for ORR relative to those of commercial Pt/C. Notably, the Mo-PdPt@Pt/ IG shows mass activity 31-fold higher than that of Pt/C and substantially maintains high activities after 10 000 cycles of intensive durability testing. The current study highlights the crucial strategies in designing the highly active and durable Pt-based octahedra and effective combination with functional graphene supports toward the synergetic effects on ORR.

Original languageEnglish
Pages (from-to)1524-1535
Number of pages12
JournalACS Applied Materials and Interfaces
Volume9
Issue number2
DOIs
Publication statusPublished - 2017 Jan 1

Fingerprint

Molybdenum
Graphite
Electrocatalysts
Graphene
Block copolymers
Reactive Oxygen Species
Oxygen
Methacrylates
Fuel cells
Durability
Metals
Methyl Ethers
Atoms
Pyrene
Oxides
Polyethylene glycols
Charge transfer
Ethers
Catalysts
Testing

Keywords

  • Core−shell structures
  • Electrocatalysts
  • Fuel cells
  • Functionalized graphene
  • Molybdenum doping
  • Multimetallic nanocrystals
  • Octahedra

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Molybdenum-doped PdPt@Pt core−shell octahedra supported by ionic block copolymer-functionalized graphene as a highly active and durable oxygen reduction electrocatalyst. / Cho, Kie Yong; Yeom, Yong Sik; Seo, Heun Young; Kumar, Pradip; Lee, Albert S.; Baek, Kyung Youl; Yoon, Ho Gyu.

In: ACS Applied Materials and Interfaces, Vol. 9, No. 2, 01.01.2017, p. 1524-1535.

Research output: Contribution to journalArticle

Cho, Kie Yong ; Yeom, Yong Sik ; Seo, Heun Young ; Kumar, Pradip ; Lee, Albert S. ; Baek, Kyung Youl ; Yoon, Ho Gyu. / Molybdenum-doped PdPt@Pt core−shell octahedra supported by ionic block copolymer-functionalized graphene as a highly active and durable oxygen reduction electrocatalyst. In: ACS Applied Materials and Interfaces. 2017 ; Vol. 9, No. 2. pp. 1524-1535.
@article{f9ce2e1c04e24767b35b044d4b7e80cc,
title = "Molybdenum-doped PdPt@Pt core−shell octahedra supported by ionic block copolymer-functionalized graphene as a highly active and durable oxygen reduction electrocatalyst",
abstract = "Development of highly active and durable electrocatalysts that can effectively electrocatalyze oxygen reduction reactions (ORR) still remains one important challenge for high-performance electrochemical conversion and storage applications such as fuel cells and metal-air batteries. Herein, we propose the combination of molybdenum-doped PdPt@Pt core−shell octahedra and the pyrene-functionalized poly(dimethylaminoethyl methacrylate)-b-poly[(ethylene glycol) methyl ether methacrylate] ionic block copolymer-functionalized reduced graphene oxide (Mo-PdPt@Pt/IG) to effectively augment the interfacial cohesion of both components using a tunable ex situ mixing strategy. The rationally designed Mo-PdPt@Pt core−shell octahedra have unique compositional benefits, including segregation of Mo atoms on the vertexes and edges of the octahedron and 2−3 shell layers of Pt atoms on a PdPt alloy core, which can provide highly active sites to the catalyst for ORR along with enhanced electrochemical stability. In addition, the ionic block copolymer functionalized graphene can facilitate intermolecular charge transfer and good stability of metal NPs, which arises from the ionic block copolymer interfacial layer. When the beneficial features of the Mo-PdPt@Pt and IG are combined, the Mo-PdPt@Pt/IG exhibits substantially enhanced activity and durability for ORR relative to those of commercial Pt/C. Notably, the Mo-PdPt@Pt/ IG shows mass activity 31-fold higher than that of Pt/C and substantially maintains high activities after 10 000 cycles of intensive durability testing. The current study highlights the crucial strategies in designing the highly active and durable Pt-based octahedra and effective combination with functional graphene supports toward the synergetic effects on ORR.",
keywords = "Core−shell structures, Electrocatalysts, Fuel cells, Functionalized graphene, Molybdenum doping, Multimetallic nanocrystals, Octahedra",
author = "Cho, {Kie Yong} and Yeom, {Yong Sik} and Seo, {Heun Young} and Pradip Kumar and Lee, {Albert S.} and Baek, {Kyung Youl} and Yoon, {Ho Gyu}",
year = "2017",
month = "1",
day = "1",
doi = "10.1021/acsami.6b13299",
language = "English",
volume = "9",
pages = "1524--1535",
journal = "ACS applied materials & interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "2",

}

TY - JOUR

T1 - Molybdenum-doped PdPt@Pt core−shell octahedra supported by ionic block copolymer-functionalized graphene as a highly active and durable oxygen reduction electrocatalyst

AU - Cho, Kie Yong

AU - Yeom, Yong Sik

AU - Seo, Heun Young

AU - Kumar, Pradip

AU - Lee, Albert S.

AU - Baek, Kyung Youl

AU - Yoon, Ho Gyu

PY - 2017/1/1

Y1 - 2017/1/1

N2 - Development of highly active and durable electrocatalysts that can effectively electrocatalyze oxygen reduction reactions (ORR) still remains one important challenge for high-performance electrochemical conversion and storage applications such as fuel cells and metal-air batteries. Herein, we propose the combination of molybdenum-doped PdPt@Pt core−shell octahedra and the pyrene-functionalized poly(dimethylaminoethyl methacrylate)-b-poly[(ethylene glycol) methyl ether methacrylate] ionic block copolymer-functionalized reduced graphene oxide (Mo-PdPt@Pt/IG) to effectively augment the interfacial cohesion of both components using a tunable ex situ mixing strategy. The rationally designed Mo-PdPt@Pt core−shell octahedra have unique compositional benefits, including segregation of Mo atoms on the vertexes and edges of the octahedron and 2−3 shell layers of Pt atoms on a PdPt alloy core, which can provide highly active sites to the catalyst for ORR along with enhanced electrochemical stability. In addition, the ionic block copolymer functionalized graphene can facilitate intermolecular charge transfer and good stability of metal NPs, which arises from the ionic block copolymer interfacial layer. When the beneficial features of the Mo-PdPt@Pt and IG are combined, the Mo-PdPt@Pt/IG exhibits substantially enhanced activity and durability for ORR relative to those of commercial Pt/C. Notably, the Mo-PdPt@Pt/ IG shows mass activity 31-fold higher than that of Pt/C and substantially maintains high activities after 10 000 cycles of intensive durability testing. The current study highlights the crucial strategies in designing the highly active and durable Pt-based octahedra and effective combination with functional graphene supports toward the synergetic effects on ORR.

AB - Development of highly active and durable electrocatalysts that can effectively electrocatalyze oxygen reduction reactions (ORR) still remains one important challenge for high-performance electrochemical conversion and storage applications such as fuel cells and metal-air batteries. Herein, we propose the combination of molybdenum-doped PdPt@Pt core−shell octahedra and the pyrene-functionalized poly(dimethylaminoethyl methacrylate)-b-poly[(ethylene glycol) methyl ether methacrylate] ionic block copolymer-functionalized reduced graphene oxide (Mo-PdPt@Pt/IG) to effectively augment the interfacial cohesion of both components using a tunable ex situ mixing strategy. The rationally designed Mo-PdPt@Pt core−shell octahedra have unique compositional benefits, including segregation of Mo atoms on the vertexes and edges of the octahedron and 2−3 shell layers of Pt atoms on a PdPt alloy core, which can provide highly active sites to the catalyst for ORR along with enhanced electrochemical stability. In addition, the ionic block copolymer functionalized graphene can facilitate intermolecular charge transfer and good stability of metal NPs, which arises from the ionic block copolymer interfacial layer. When the beneficial features of the Mo-PdPt@Pt and IG are combined, the Mo-PdPt@Pt/IG exhibits substantially enhanced activity and durability for ORR relative to those of commercial Pt/C. Notably, the Mo-PdPt@Pt/ IG shows mass activity 31-fold higher than that of Pt/C and substantially maintains high activities after 10 000 cycles of intensive durability testing. The current study highlights the crucial strategies in designing the highly active and durable Pt-based octahedra and effective combination with functional graphene supports toward the synergetic effects on ORR.

KW - Core−shell structures

KW - Electrocatalysts

KW - Fuel cells

KW - Functionalized graphene

KW - Molybdenum doping

KW - Multimetallic nanocrystals

KW - Octahedra

UR - http://www.scopus.com/inward/record.url?scp=85013320260&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85013320260&partnerID=8YFLogxK

U2 - 10.1021/acsami.6b13299

DO - 10.1021/acsami.6b13299

M3 - Article

AN - SCOPUS:85013320260

VL - 9

SP - 1524

EP - 1535

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

SN - 1944-8244

IS - 2

ER -