Journal
NATURE CHEMISTRY
Volume 2, Issue 6, Pages 454-460Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.623
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Funding
- Department of Energy, Office of Basic Energy Sciences
- National Science Foundation [729722]
- German National Science Foundation (Deutsche Forschungsgemeinschaft)
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Department of Energy's Office of Biological and Environmental Research
- ORNL's SHaRE User Program
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Electrocatalysis will play a key role in future energy conversion and storage technologies, such as water electrolysers, fuel cells and metal-air batteries. Molecular interactions between chemical reactants and the catalytic surface control the activity and efficiency, and hence need to be optimized; however, generalized experimental strategies to do so are scarce. Here we show how lattice strain can be used experimentally to tune the catalytic activity of dealloyed bimetallic nanoparticles for the oxygen-reduction reaction, a key barrier to the application of fuel cells and metal-air batteries. We demonstrate the core-shell structure of the catalyst and clarify the mechanistic origin of its activity. The platinum-rich shell exhibits compressive strain, which results in a shift of the electronic band structure of platinum and weakening chemisorption of oxygenated species. We combine synthesis, measurements and an understanding of strain from theory to generate a reactivity-strain relationship that provides guidelines for tuning electrocatalytic activity.
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