Facet-Dependent Deposition of Highly Strained Alloyed Shells on Intermetallic Nanoparticles for Enhanced Electrocatalysis

Chenyu Wang; Xiahan Sang; Jocelyn T.L. Gamler; Dennis P. Chen; Raymond R. Unocic; Sara E. Skrabalak

doi:10.1021/acs.nanolett.7b02239

Facet-Dependent Deposition of Highly Strained Alloyed Shells on Intermetallic Nanoparticles for Enhanced Electrocatalysis

Chenyu Wang, Xiahan Sang, Jocelyn T.L. Gamler, Dennis P. Chen, Raymond R. Unocic, Sara E. Skrabalak

Materials MicroAnalysis

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

91 Scopus citations

Abstract

Surface strains can enhance the performance of platinum-based core@shell electrocatalysts for the oxygen reduction reaction (ORR). Bimetallic core@shell nanoparticles (NPs) are widely studied nanocatalysts but often have limited lattice mismatch and surface compositions; investigations of core@shell NPs with greater compositional complexity and lattice misfit are in their infancy. Here, a new class of multimetallic NPs composed of intermetallic cores and random alloy shells is reported. Specifically, face-centered cubic Pt-Cu random alloy shells were deposited on PdCu B2 intermetallic seeds in a facet-dependent manner, giving rise to faceted core@shell NPs with highly strained surfaces. High-resolution transmission electron microscopy revealed orientation-dependent surface strains, where the compressive strains were greater on Pt-Cu {200} than {111} facets. These core@shell NPs provide higher specific area and mass activities for the ORR when compared to conventional Pt-Cu NPs. Moreover, these intermetallic@random alloy NPs displayed high endurance, undergoing 10,000 cycles with only a slight decay in activity and no apparent structural changes.

Original language	English
Pages (from-to)	5526-5532
Number of pages	7
Journal	Nano Letters
Volume	17
Issue number	9
DOIs	https://doi.org/10.1021/acs.nanolett.7b02239
State	Published - Sep 13 2017

Funding

We acknowledge financial support from the U.S. Department of Energy (Basic Energy Sciences) through an Early Career Award Grant (DE-SC0010489). Access to the X-ray powder diffractometer and the XPS was provided by NSF CHE CRIF-1048613 and DMR MRI-1126394, respectively. HAADF-STEM EDX mapping was conducted at Nanoscale Characterization Facility and Electron Microscopy Center at IU. Aberration-corrected STEM was conducted as part of a user proposal at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy Office of Science User Facility (X.S. and R.R.U.). S.E.S is also supported through the Camille Dreyfus Teacher Scholar Program. D.P.C. is thankful for the financial support provided by the President’s Diversity Dissertation Fellowship.

Funders	Funder number
Camille Dreyfus
National Science Foundation	DMR MRI-1126394, CHE CRIF-1048613
U.S. Department of Energy
Basic Energy Sciences	DE-SC0010489

Keywords

Pt-M nanoparticles
core-shell
lattice misfit
oxygen reduction reaction
seeded growth
surface strains

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10.1021/acs.nanolett.7b02239

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title = "Facet-Dependent Deposition of Highly Strained Alloyed Shells on Intermetallic Nanoparticles for Enhanced Electrocatalysis",

abstract = "Surface strains can enhance the performance of platinum-based core@shell electrocatalysts for the oxygen reduction reaction (ORR). Bimetallic core@shell nanoparticles (NPs) are widely studied nanocatalysts but often have limited lattice mismatch and surface compositions; investigations of core@shell NPs with greater compositional complexity and lattice misfit are in their infancy. Here, a new class of multimetallic NPs composed of intermetallic cores and random alloy shells is reported. Specifically, face-centered cubic Pt-Cu random alloy shells were deposited on PdCu B2 intermetallic seeds in a facet-dependent manner, giving rise to faceted core@shell NPs with highly strained surfaces. High-resolution transmission electron microscopy revealed orientation-dependent surface strains, where the compressive strains were greater on Pt-Cu {200} than {111} facets. These core@shell NPs provide higher specific area and mass activities for the ORR when compared to conventional Pt-Cu NPs. Moreover, these intermetallic@random alloy NPs displayed high endurance, undergoing 10,000 cycles with only a slight decay in activity and no apparent structural changes.",

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N2 - Surface strains can enhance the performance of platinum-based core@shell electrocatalysts for the oxygen reduction reaction (ORR). Bimetallic core@shell nanoparticles (NPs) are widely studied nanocatalysts but often have limited lattice mismatch and surface compositions; investigations of core@shell NPs with greater compositional complexity and lattice misfit are in their infancy. Here, a new class of multimetallic NPs composed of intermetallic cores and random alloy shells is reported. Specifically, face-centered cubic Pt-Cu random alloy shells were deposited on PdCu B2 intermetallic seeds in a facet-dependent manner, giving rise to faceted core@shell NPs with highly strained surfaces. High-resolution transmission electron microscopy revealed orientation-dependent surface strains, where the compressive strains were greater on Pt-Cu {200} than {111} facets. These core@shell NPs provide higher specific area and mass activities for the ORR when compared to conventional Pt-Cu NPs. Moreover, these intermetallic@random alloy NPs displayed high endurance, undergoing 10,000 cycles with only a slight decay in activity and no apparent structural changes.

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Facet-Dependent Deposition of Highly Strained Alloyed Shells on Intermetallic Nanoparticles for Enhanced Electrocatalysis

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