Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion
Abstract
Design of cost-effective electrocatalysts with enhanced stability and activity is of paramount importance for the next generation of energy conversion systems, including fuel cells and electrolyzers. However, electrocatalytic materials generally improve one of these properties at the expense of the other. Here, using Density Functional Theory calculations and electrochemical surface science measurements, we explore atomic-level features of ultrathin (hydroxy)oxide films on transition metal substrates and demonstrate that these films exhibit both excellent stability and activity for electrocatalytic applications. The films adopt structures with stabilities that significantly exceed bulk Pourbaix limits, including stoichiometries not found in bulk and properties that are tunable by controlling voltage, film composition, and substrate identity. Using nickel (hydroxy)oxide/Pt(111) as an example, we further show how the films enhance activity for hydrogen evolution through a bifunctional effect. Finally, the results suggest design principles for a new class of electrocatalysts with simultaneously enhanced stability and activity for energy conversion.
- Authors:
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences and Engineering Division; Early Career Award; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Energy Research Scientific Computing Center (NERSC)
- OSTI Identifier:
- 1364140
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Energy
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 6; Journal ID: ISSN 2058-7546
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zeng, Zhenhua, Chang, Kee-Chul, Kubal, Joseph, Markovic, Nenad M., and Greeley, Jeffrey. Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion. United States: N. p., 2017.
Web. doi:10.1038/nenergy.2017.70.
Zeng, Zhenhua, Chang, Kee-Chul, Kubal, Joseph, Markovic, Nenad M., & Greeley, Jeffrey. Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion. United States. https://doi.org/10.1038/nenergy.2017.70
Zeng, Zhenhua, Chang, Kee-Chul, Kubal, Joseph, Markovic, Nenad M., and Greeley, Jeffrey. Mon .
"Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion". United States. https://doi.org/10.1038/nenergy.2017.70. https://www.osti.gov/servlets/purl/1364140.
@article{osti_1364140,
title = {Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion},
author = {Zeng, Zhenhua and Chang, Kee-Chul and Kubal, Joseph and Markovic, Nenad M. and Greeley, Jeffrey},
abstractNote = {Design of cost-effective electrocatalysts with enhanced stability and activity is of paramount importance for the next generation of energy conversion systems, including fuel cells and electrolyzers. However, electrocatalytic materials generally improve one of these properties at the expense of the other. Here, using Density Functional Theory calculations and electrochemical surface science measurements, we explore atomic-level features of ultrathin (hydroxy)oxide films on transition metal substrates and demonstrate that these films exhibit both excellent stability and activity for electrocatalytic applications. The films adopt structures with stabilities that significantly exceed bulk Pourbaix limits, including stoichiometries not found in bulk and properties that are tunable by controlling voltage, film composition, and substrate identity. Using nickel (hydroxy)oxide/Pt(111) as an example, we further show how the films enhance activity for hydrogen evolution through a bifunctional effect. Finally, the results suggest design principles for a new class of electrocatalysts with simultaneously enhanced stability and activity for energy conversion.},
doi = {10.1038/nenergy.2017.70},
journal = {Nature Energy},
number = 6,
volume = 2,
place = {United States},
year = {Mon May 08 00:00:00 EDT 2017},
month = {Mon May 08 00:00:00 EDT 2017}
}
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