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Title: Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction

Abstract

Pt-based materials are the state-of-the-art catalysts for oxygen reduction reaction (ORR), but their high cost and scarcity remain the major obstacles for large-scale applications in renewable energy industries. To produce efficient ORR catalysts with low Pt content, PtNi porous films (PFs) with sufficiently exposed Pt active sites were rationally designed through a programmable approach combining electrochemical bottom-up (electrodeposition) and topdown (anodization) processes. The unique dynamic oxygen-bubble template (DOBT) programmably controlled by square-wave potential was utilized to tune the catalyst morphology and expose Pt active facets in PtNi PFs. Here, the surface-bounded species such as hydroxyl anions (OH*, *=surface site) on the exposed PtNi PFs surfaces were adjusted by the applied anodic voltage, further affecting the dynamic oxygen (O 2) bubbles adsorption on Pt. As a result, PtNi PF with enriched Pt (111) facets (denoted as Pt 3.5%Ni PF) was obtained, showing prominent ORR activity with an onset potential of 0.92 V (vs. RHE) at an ultra-low Pt loading (0.015 mg cm -2). The adsorbed OHads coverage estimation shows fewer OHads on Pt 3.5%Ni PF than other PtNi PFs, indicating that enriched Pt (111) facets in the catalysts enable facilitated O 2 adsorption for oxygen reduction and thus leading to superiormore » ORR activity« less

Authors:
 [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Central Florida, Orlando, FL (United States). NanoScience Technology Center, Dept. of Materials Science and Engineering, Energy Conversion and Propulsion Cluster
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Sciences Directorate
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1577057
Report Number(s):
PNNL-SA-147087
Journal ID: ISSN 1433-7851; ANIE
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 44; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; low Pt loading; dynamic oxygen-bubble template; porous film; facet-selective; oxygen reduction

Citation Formats

Wang, Guanzhi, Yang, Zhenzhong, Du, Yingge, and Yang, Yang. Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction. United States: N. p., 2019. Web. doi:10.1002/anie.201907322.
Wang, Guanzhi, Yang, Zhenzhong, Du, Yingge, & Yang, Yang. Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction. United States. doi:10.1002/anie.201907322.
Wang, Guanzhi, Yang, Zhenzhong, Du, Yingge, and Yang, Yang. Mon . "Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction". United States. doi:10.1002/anie.201907322.
@article{osti_1577057,
title = {Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction},
author = {Wang, Guanzhi and Yang, Zhenzhong and Du, Yingge and Yang, Yang},
abstractNote = {Pt-based materials are the state-of-the-art catalysts for oxygen reduction reaction (ORR), but their high cost and scarcity remain the major obstacles for large-scale applications in renewable energy industries. To produce efficient ORR catalysts with low Pt content, PtNi porous films (PFs) with sufficiently exposed Pt active sites were rationally designed through a programmable approach combining electrochemical bottom-up (electrodeposition) and topdown (anodization) processes. The unique dynamic oxygen-bubble template (DOBT) programmably controlled by square-wave potential was utilized to tune the catalyst morphology and expose Pt active facets in PtNi PFs. Here, the surface-bounded species such as hydroxyl anions (OH*, *=surface site) on the exposed PtNi PFs surfaces were adjusted by the applied anodic voltage, further affecting the dynamic oxygen (O2) bubbles adsorption on Pt. As a result, PtNi PF with enriched Pt (111) facets (denoted as Pt3.5%Ni PF) was obtained, showing prominent ORR activity with an onset potential of 0.92 V (vs. RHE) at an ultra-low Pt loading (0.015 mg cm-2). The adsorbed OHads coverage estimation shows fewer OHads on Pt3.5%Ni PF than other PtNi PFs, indicating that enriched Pt (111) facets in the catalysts enable facilitated O2 adsorption for oxygen reduction and thus leading to superior ORR activity},
doi = {10.1002/anie.201907322},
journal = {Angewandte Chemie (International Edition)},
number = 44,
volume = 58,
place = {United States},
year = {2019},
month = {9}
}

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