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Imaging the strain evolution of a platinum nanoparticle under electrochemical control

Nature Materials volume 22, pages 754–761 (2023)Cite this article

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Abstract

Surface strain is widely employed in gas phase catalysis and electrocatalysis to control the binding energies of adsorbates on active sites. However, in situ or operando strain measurements are experimentally challenging, especially on nanomaterials. Here we exploit coherent diffraction at the new fourth-generation Extremely Brilliant Source of the European Synchrotron Radiation Facility to map and quantify strain within individual Pt catalyst nanoparticles under electrochemical control. Three-dimensional nanoresolution strain microscopy, together with density functional theory and atomistic simulations, show evidence of heterogeneous and potential-dependent strain distribution between highly coordinated ({100} and {111} facets) and undercoordinated atoms (edges and corners), as well as evidence of strain propagation from the surface to the bulk of the nanoparticle. These dynamic structural relationships directly inform the design of strain-engineered nanocatalysts for energy storage and conversion applications.

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Fig. 1: Scheme of the experimental setup to image strain distribution onto a single Pt nanoparticle.
Fig. 2: Influence of electrode potential on surface strain (ε002).
Fig. 3: Distributions of surface versus bulk strain, facet versus edge/corner strain and top/bottom facet versus side facet strain as a function of electrode potential.
Fig. 4: Modelling indicates that strain gradients are largely independent of crystallite size.
Fig. 5: Adsorption configurations of HSO4 on Pt model morphological features (periodic slab modes) and their associated strain response along the [002] direction.
Fig. 6: Mechanical accommodation of a Pt nanoparticle following (bi)sulfate ion adsorption.

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Data availability

When published the data will be uploaded to the CXI database (https://www.cxidb.org) and is available here (https://data.esrf.fr/doi/10.15151/ESRF-DC-1104468572).

Code availability

The code used can be found in refs. 42,45,52.

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Acknowledgements

We thank the European Synchrotron Radiation Facility for allocating beamtime, and the ID01 beamline staff for their excellent support during measurements. This project received funding from the European Research Council under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 818823 to M.-I.R.). The authors thank É. Gaudry, P. Sautet and T. Deutsch for fruitful discussions on DFT simulations. The authors also thank B. Gilles for his help and advice during the preparation of samples, and J. P. Hofmann and E. J. M. Hensen for insightful advice.

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Authors and Affiliations

  1. Univ. Grenoble Alpes, CEA Grenoble, IRIG, MEM, NRX, Grenoble, France

    Clément Atlan, Corentin Chatelier, Maxime Dupraz, Ni Li, Joël Eymery & Marie-Ingrid Richard

  2. ESRF – The European Synchrotron, Grenoble, France

    Clément Atlan, Corentin Chatelier, Isaac Martens, Maxime Dupraz, Ni Li, Steven J. Leake, Tobias U. Schülli & Marie-Ingrid Richard

  3. Univ. Grenoble Alpes, Univ. Savoie Mont Blanc, CNRS, Grenoble INP, LEPMI, Grenoble, France

    Clément Atlan, Arnaud Viola & Frédéric Maillard

  4. Laboratory for Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, Eindhoven, the Netherlands

    Lu Gao

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Contributions

M.-I.R. and F.M. conceived and designed experiments. L.G. developed the electrochemical cell and performed Pt/GC synthesis. C.A., I.M., M.D., N.L., S.J.L., T.U.S., A.V., F.M. and M.-I.R. performed in situ BCDI measurements. C.A., C.C. and M.-I.R. analysed data. C.C. performed MSS and DFT calculations. C.A. wrote the first version of the manuscript. C.A., C.C., I.M., J.E., F.M. and M.-I.R. revised the manuscript.

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Correspondence to Clément Atlan, Corentin Chatelier, Frédéric Maillard or Marie-Ingrid Richard.

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Atlan, C., Chatelier, C., Martens, I. et al. Imaging the strain evolution of a platinum nanoparticle under electrochemical control. Nat. Mater. 22, 754–761 (2023). https://doi.org/10.1038/s41563-023-01528-x

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