Tunable intrinsic strain in two-dimensional transition metal electrocatalysts
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- 21 February 2019
- journal article
- research article
- Published by American Association for the Advancement of Science (AAAS) in Science
- Vol. 363 (6429), 870-+
- https://doi.org/10.1126/science.aat8051
Abstract
Tuning surface strain is a powerful strategy for tailoring the reactivity of metal catalysts. Traditionally, surface strain is imposed by external stress from a heterogeneous substrate, but the effect is often obscured by interfacial reconstructions and nanocatalyst geometries. Here, we report on a strategy to resolve these problems by exploiting intrinsic surface stresses in two-dimensional transition metal nanosheets. Density functional theory calculations indicate that attractive interactions between surface atoms lead to tensile surface stresses that exert a pressure on the order of 10(5) atmospheres on the surface atoms and impart up to 10% compressive strain, with the exact magnitude inversely proportional to the nanosheet thickness. Atomic-level control of thickness thus enables generation and fine-tuning of intrinsic strain to optimize catalytic reactivity, which was confirmed experimentally on Pd(110) nanosheets for the oxygen reduction and hydrogen evolution reactions, with activity enhancements that were more than an order of magnitude greater than those of their nanoparticle counterparts.Keywords
Funding Information
- National Science Foundation (CBET-1437219)
- National Science Foundation (CBET 1159240, DMR-1420620, and DMR- 1506535.)
- U.S. Department of Energy (DE-SC0010379)
- U.S. Department of Energy (DE-EE0007270)
- U.S. Department of Energy (E-AC02-06CH11357)
This publication has 62 references indexed in Scilit:
- Combining theory and experiment in electrocatalysis: Insights into materials designScience, 2017
- Energy and fuels from electrochemical interfacesNature Materials, 2016
- Biaxially strained PtPb/Pt core/shell nanoplate boosts oxygen reduction catalysisScience, 2016
- Ultrafine jagged platinum nanowires enable ultrahigh mass activity for the oxygen reduction reactionScience, 2016
- Platinum-based nanocages with subnanometer-thick walls and well-defined, controllable facetsScience, 2015
- Element-specific anisotropic growth of shaped platinum alloy nanocrystalsScience, 2014
- Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic SurfacesScience, 2014
- Freestanding palladium nanosheets with plasmonic and catalytic propertiesNature Nanotechnology, 2010
- Role of Strain and Ligand Effects in the Modification of the Electronic and Chemical Properties of Bimetallic SurfacesPhysical Review Letters, 2004
- Effect of Strain on the Reactivity of Metal SurfacesPhysical Review Letters, 1998