Enhancing ORR Performance of Bimetallic PdAg Electrocatalysts by Designing Interactions between Pd and Ag

Luis E. Betancourt; Arnulfo Rojas-Pérez; Ivan Orozco; Anatoly I. Frenkel; Yuanyuan Li; Kotaro Sasaki; Sanjaya D. Senanayake; Carlos R. Cabrera

doi:10.1021/acsaem.9b01920

Enhancing ORR Performance of Bimetallic PdAg Electrocatalysts by Designing Interactions between Pd and Ag

Luis E. Betancourt, Arnulfo Rojas-Pérez, Ivan Orozco, Anatoly I. Frenkel, Yuanyuan Li, Kotaro Sasaki, Sanjaya D. Senanayake, Carlos R. Cabrera

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

46 Scopus citations

Abstract

Precise tuning of the electronic properties of Ag/C using under potentially deposited (UPD) Cu and subsequent galvanic displacement to deposit atomically dispersed loading of Pd resulted in a robust bimetallic alloy with significant activity for the oxygen reduction reaction in alkaline media. The specific design of the catalyst and atomic arrangement of Pd-Ag outperforms conventional Pd/C and Ag/C commercial catalysts. The ORR activity of Pd deposited onto Ag/C was determined on the basis of rotating disk electrode voltammetry studies, showing a 2-fold increase in Pd mass activities compared to results obtained using Pd/C. While scanning transmission electron microcopy (STEM) coupled with electron energy loss spectroscopy (EELS) probed the uniformity of the nanoparticles, the origin of the outstanding activity was traced to the structural properties of the Pd-Ag interface as shown by X-ray absorption spectroscopy (XAS), along with X-ray photoelectron spectroscopy (XPS). Segregation of metals with a suitable geometric arrangement of the Ag to Pd ratio at the interface resulted in an increased performance where the active sites were key steps of oxygen bond breaking.

Original language	English
Pages (from-to)	2342-2349
Number of pages	8
Journal	ACS Applied Energy Materials
Volume	3
Issue number	3
DOIs	https://doi.org/10.1021/acsaem.9b01920
State	Published - Mar 23 2020
Externally published	Yes

Funding

This work was financially supported by the NSF-CREST Center for Innovation, Research and Education in Environmental Nanotechnology Grant HRD-1736093 and NSF-PREM Center for Interfacial Electrochemistry of Energy Materials Grant DMR-1827622. EXAFS analysis and modeling of Ag–Pd interactions by AIF were supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award DE-SC0012573. This research used resources of the Center for Functional Nanomaterials (CFN), which is a U.S. DOE Office of Science Facility, at Brookhaven National Laboratory (BNL) under Contract DE-SC0012704. We thank Kim Kisslinger (CFN-BNL) for assistance with the TEM images. This research used resources of beamline 8-ID and 8-BM of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract DE-SC0012704.

Funders	Funder number
NSF-CREST Center for Innovation, Research and Education in Environmental Nanotechnology	HRD-1736093
NSF-PREM	DMR-1827622
National Science Foundation	1827622, 1736093
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-SC0012573
Brookhaven National Laboratory	DE-SC0012704

Keywords

Ag/Pd bimatallic nanoparticles
Cu UPD
electrocatalysis
galvanic displacement
oxygen reduction

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10.1021/acsaem.9b01920

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title = "Enhancing ORR Performance of Bimetallic PdAg Electrocatalysts by Designing Interactions between Pd and Ag",

abstract = "Precise tuning of the electronic properties of Ag/C using under potentially deposited (UPD) Cu and subsequent galvanic displacement to deposit atomically dispersed loading of Pd resulted in a robust bimetallic alloy with significant activity for the oxygen reduction reaction in alkaline media. The specific design of the catalyst and atomic arrangement of Pd-Ag outperforms conventional Pd/C and Ag/C commercial catalysts. The ORR activity of Pd deposited onto Ag/C was determined on the basis of rotating disk electrode voltammetry studies, showing a 2-fold increase in Pd mass activities compared to results obtained using Pd/C. While scanning transmission electron microcopy (STEM) coupled with electron energy loss spectroscopy (EELS) probed the uniformity of the nanoparticles, the origin of the outstanding activity was traced to the structural properties of the Pd-Ag interface as shown by X-ray absorption spectroscopy (XAS), along with X-ray photoelectron spectroscopy (XPS). Segregation of metals with a suitable geometric arrangement of the Ag to Pd ratio at the interface resulted in an increased performance where the active sites were key steps of oxygen bond breaking.",

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author = "Betancourt, {Luis E.} and Arnulfo Rojas-P{\'e}rez and Ivan Orozco and Frenkel, {Anatoly I.} and Yuanyuan Li and Kotaro Sasaki and Senanayake, {Sanjaya D.} and Cabrera, {Carlos R.}",

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AU - Frenkel, Anatoly I.

AU - Li, Yuanyuan

AU - Sasaki, Kotaro

AU - Senanayake, Sanjaya D.

AU - Cabrera, Carlos R.

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AB - Precise tuning of the electronic properties of Ag/C using under potentially deposited (UPD) Cu and subsequent galvanic displacement to deposit atomically dispersed loading of Pd resulted in a robust bimetallic alloy with significant activity for the oxygen reduction reaction in alkaline media. The specific design of the catalyst and atomic arrangement of Pd-Ag outperforms conventional Pd/C and Ag/C commercial catalysts. The ORR activity of Pd deposited onto Ag/C was determined on the basis of rotating disk electrode voltammetry studies, showing a 2-fold increase in Pd mass activities compared to results obtained using Pd/C. While scanning transmission electron microcopy (STEM) coupled with electron energy loss spectroscopy (EELS) probed the uniformity of the nanoparticles, the origin of the outstanding activity was traced to the structural properties of the Pd-Ag interface as shown by X-ray absorption spectroscopy (XAS), along with X-ray photoelectron spectroscopy (XPS). Segregation of metals with a suitable geometric arrangement of the Ag to Pd ratio at the interface resulted in an increased performance where the active sites were key steps of oxygen bond breaking.

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Enhancing ORR Performance of Bimetallic PdAg Electrocatalysts by Designing Interactions between Pd and Ag

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