Predicting the oxygen-binding properties of platinum nanoparticle ensembles by combining high-precision electron microscopy and density functional theory

Journal article

Many studies of heterogeneous catalysis, both experimental and computational, make use of idealized structures such as extended surfaces or regular polyhedral nanoparticles. This simplification neglects the morphological diversity in real commercial oxygen reduction reaction (ORR) catalysts used in fuel-cell cathodes. Here we introduce an approach that combines 3D nanoparticle structures obtained from high-throughput high-precision electron microscopy with density functional theory. Discrepancies between experimental observations and cuboctahedral/truncated-octahedral particles are revealed and discussed using a range of widely used descriptors, such as electron-density, d-band centers, and generalized coordination numbers. We use this new approach to determine the optimum particle size for which both detrimental surface roughness and particle shape effects are minimized.

Authors: Aarons, J; Jones, L; Varambhia, A; MacArthur, K; Ozkaya, D

• Publication status: Published
• Peer review status: Peer reviewed
• Publisher: American Chemical Society
• Journal: Nano Letters
• Volume: 17
• Issue: 7
• Pages: 4003-4012
• Publication date: 2017-06-23
• Acceptance date: 2017-06-23
• DOI: 10.1021/acs.nanolett.6b04799
• EISSN: 1530-6992
• ISSN: 1530-6984
• Language: English
• Keywords: ADF STEM; density functional theory; fuel cells; heterogeneous catalysis