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Title: Correlating the electrocatalytic stability of platinum monolayer catalysts with their structural evolution in the oxygen reduction reaction

Platinum monolayer (Pt ML) core–shell electrocatalysts for the oxygen reduction reaction (ORR) have attracted great attention because of their exceptional activity and stability for promising practical applications in fuel cells. In this paper, we describe our in-depth investigation of the relationship between the ORR activity and structure of the Pt ML/Pd/C catalyst during the stability test. By virtue of the rotating disk electrode technique, an accelerated degradation test with the potential window of 0.65 to 1.05 V was applied to the Pt ML/Pd/C to interrogate its long-term reliability in the ORR, the change of its electrochemical surface area, and its surface composition and components. The Pt ML/Pd/C catalyst displayed a volcano-like mass/dollar activity profile in the stability test up to 100k cycles. The overall loss of the activity was recorded to be as low as 17% of the initial value. The ORR activity increased in the initial 20k cycles because the freshly prepared Pt ML did not entirely encompass the whole Pd core, but it was integrated to a full coverage with a more stable configuration during the potential cycling owing to its self-healing property. Then, the activity decreased at a much slower rate than the standard Pt/C because themore » Pd–Pt core–shell structure due to its structural self-retaining property remained intact and impeded the electrochemical Ostwald ripening of the entire particles. Changes in the morphology and configuration of Pt ML were mapped by combining our experimental investigation with model analyses. Finally, the proposed self-healing and self-retaining mechanisms account for the structure-dependent stability in the ORR and play cornerstone roles in formulating ORR core–shell electrocatalysts.« less
Authors:
ORCiD logo [1] ;  [2] ;  [2] ;  [2] ; ORCiD logo [3] ; ORCiD logo [3] ;  [3] ; ORCiD logo [3] ; ORCiD logo [3] ; ORCiD logo [2] ;  [2]
  1. Harbin Institute of Technology (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Harbin Institute of Technology (China)
Publication Date:
Report Number(s):
BNL-209808-2018-JAAM
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 42; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1488522
Alternate Identifier(s):
OSTI ID: 1477520

Chen, Guangyu, Kuttiyiel, Kurian A., Li, Meng, Su, Dong, Du, Lei, Du, Chunyu, Gao, Yunzhi, Fei, Weidong, Yin, Geping, Sasaki, Kotaro, and Adzic, Radoslav R.. Correlating the electrocatalytic stability of platinum monolayer catalysts with their structural evolution in the oxygen reduction reaction. United States: N. p., Web. doi:10.1039/C8TA06686H.
Chen, Guangyu, Kuttiyiel, Kurian A., Li, Meng, Su, Dong, Du, Lei, Du, Chunyu, Gao, Yunzhi, Fei, Weidong, Yin, Geping, Sasaki, Kotaro, & Adzic, Radoslav R.. Correlating the electrocatalytic stability of platinum monolayer catalysts with their structural evolution in the oxygen reduction reaction. United States. doi:10.1039/C8TA06686H.
Chen, Guangyu, Kuttiyiel, Kurian A., Li, Meng, Su, Dong, Du, Lei, Du, Chunyu, Gao, Yunzhi, Fei, Weidong, Yin, Geping, Sasaki, Kotaro, and Adzic, Radoslav R.. 2018. "Correlating the electrocatalytic stability of platinum monolayer catalysts with their structural evolution in the oxygen reduction reaction". United States. doi:10.1039/C8TA06686H.
@article{osti_1488522,
title = {Correlating the electrocatalytic stability of platinum monolayer catalysts with their structural evolution in the oxygen reduction reaction},
author = {Chen, Guangyu and Kuttiyiel, Kurian A. and Li, Meng and Su, Dong and Du, Lei and Du, Chunyu and Gao, Yunzhi and Fei, Weidong and Yin, Geping and Sasaki, Kotaro and Adzic, Radoslav R.},
abstractNote = {Platinum monolayer (PtML) core–shell electrocatalysts for the oxygen reduction reaction (ORR) have attracted great attention because of their exceptional activity and stability for promising practical applications in fuel cells. In this paper, we describe our in-depth investigation of the relationship between the ORR activity and structure of the PtML/Pd/C catalyst during the stability test. By virtue of the rotating disk electrode technique, an accelerated degradation test with the potential window of 0.65 to 1.05 V was applied to the PtML/Pd/C to interrogate its long-term reliability in the ORR, the change of its electrochemical surface area, and its surface composition and components. The PtML/Pd/C catalyst displayed a volcano-like mass/dollar activity profile in the stability test up to 100k cycles. The overall loss of the activity was recorded to be as low as 17% of the initial value. The ORR activity increased in the initial 20k cycles because the freshly prepared PtML did not entirely encompass the whole Pd core, but it was integrated to a full coverage with a more stable configuration during the potential cycling owing to its self-healing property. Then, the activity decreased at a much slower rate than the standard Pt/C because the Pd–Pt core–shell structure due to its structural self-retaining property remained intact and impeded the electrochemical Ostwald ripening of the entire particles. Changes in the morphology and configuration of PtML were mapped by combining our experimental investigation with model analyses. Finally, the proposed self-healing and self-retaining mechanisms account for the structure-dependent stability in the ORR and play cornerstone roles in formulating ORR core–shell electrocatalysts.},
doi = {10.1039/C8TA06686H},
journal = {Journal of Materials Chemistry. A},
number = 42,
volume = 6,
place = {United States},
year = {2018},
month = {9}
}

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