Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction

Wang, Guanzhi; Yang, Zhenzhong; Du, Yingge; Yang, Yang

doi:10.1002/anie.201907322

Programmable Exposure of Pt Active Facets for Efficient Oxygen Reduction

Journal Article · Mon Sep 02 00:00:00 EDT 2019 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201907322· OSTI ID:1577057

Wang, Guanzhi ^[1]; Yang, Zhenzhong ^[2]; ^[2]; ^[1]

Univ. of Central Florida, Orlando, FL (United States). NanoScience Technology Center, Dept. of Materials Science and Engineering, Energy Conversion and Propulsion Cluster
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Sciences Directorate

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 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 O₂ adsorption for oxygen reduction and thus leading to superior ORR activity

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1577057

Report Number(s):: PNNL-SA--147087

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 44 Vol. 58; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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