Title: Composition–Structure–Activity Correlation of Platinum–Ruthenium Nanoalloy Catalysts for Ethanol Oxidation Reaction

Abstract

Understanding the evolution of the composition and atomic structure of nanoalloy catalysts in the ethanol oxidation reaction (EOR) is essential for the design of active and robust catalysts for direct ethanol fuel cells. This article describes a study of carbon-supported platinum–ruthenium electrocatalysts (PtRu/C) with different bimetallic compositions and their activities in the EOR, an important anode reaction in direct ethanol fuel cells (DEFCs). The study focused on establishing the relationship between the catalyst’s composition, atomic structure, and catalytic activity for the EOR. Ex situ and in situ synchrotron high-energy X-ray diffraction (HE-XRD) experiments coupled with atomic pair distribution function (PDF) analysis and in situ energy-dispersive X-ray (EDX) analysis were employed to probe the composition and structural evolution of the catalysts during the in situ EOR inside a membrane electrode assembly (MEA) in the fuel cell. The results revealed an intriguing composition–structure–activity relationship for the PtRu electrocatalysts under EOR experimental conditions. In particular, the alloy with a Pt/Ru ratio of ~50:50 was found to exhibit a maximum EOR activity as a function of the bimetallic composition. This composition–activity relationship coincides with the relationship between the Pt interatomic distances and coordination numbers and the bimetallic composition. Notably, the catalytic activities of themore » PtRu electrocatalysts showed a significant improvement during the EOR, which can be related to atomic-level structural changes in the nanoalloys occurring during the EOR, as indicated by in situ HE-XRD/PDF/EDX data. Here, the findings shed some new light on the mechanism of the ethanol oxidation reaction over bimetallic alloy nanocatalysts, which is important for the rational design and synthesis of active nanoalloy catalysts for DEFCs.« less

Authors:

Zhao, Yinguang ^[1]; Maswadeh, Yazan ^[2]; Shan, Shiyao ^[1]; Cronk, Hannah ^[1]; Skeete, Zakiya ^[1]; Prasai, Binay ^[2]; Luo, Jin ^[1]; Petkov, Valeri  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-6392-7589"

Zhong, Chuan-Jian  ^[1]

• Search DOE PAGES for author "Zhong, Chuan-Jian"
• Search DOE PAGES for ORCID "0000-0003-0746-250X"

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+ Show Author Affiliations

1. State Univ. of New York, Binghamton, NY (United States)
2. Central Michigan Univ., Mt. Pleasant, MI (United States)

Publication Date:

Thu Aug 03 00:00:00 EDT 2017

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:

1437478

Grant/Contract Number:  

AC02-06CH11357; SC0006877; CHE 1566283

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Physical Chemistry. C

Additional Journal Information:

Journal Volume: 121; Journal Issue: 32; Journal ID: ISSN 1932-7447

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

ENGLISH

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; platinum; bioethanol; catalysts; catalytic activity; fuel cells