Single alloy nanoparticle x-ray imaging during a catalytic reaction

Young Yong Kim, Thomas F. Keller, Tiago J. Goncalves, Manuel Abuin, Henning Runge, Luca Gelisio, Jerome Carnis, Vedran Vonk, Philipp N. Plessow, Ivan A. Vartaniants, Andreas Stierle

Research output: Contribution to journalArticlepeer-review

Abstract

The imaging of active nanoparticles represents a milestone in decoding heterogeneous catalysts’ dynamics. We report the facet-resolved, surface strain state of a single PtRh alloy nanoparticle on SrTiO3 determined by coherent x-ray diffraction imaging under catalytic reaction conditions. Density functional theory calculations allow us to correlate the facet surface strain state to its reaction environment–dependent chemical composition. We find that the initially Pt-terminated nanoparticle surface gets Rh-enriched under CO oxidation reaction conditions. The local composition is facet orientation dependent, and the Rh enrichment is nonreversible under subsequent CO reduction. Tracking facet-resolved strain and composition under operando conditions is crucial for a rational design of more efficient heterogeneous catalysts with tailored activity, selectivity, and lifetime.

Original languageEnglish
Article numbereabh0757
JournalScience Advances
Volume7
Issue number40
DOIs
Publication statusPublished - 2021 Oct

Bibliographical note

Funding Information:
Funding from the European Union H2020 project ?Nanoscience Foundries and Fine Analysis? (NFFA), grant no. 654360, from BMBF grant 5K13WC3 (PT-DESY), and from DFG SFB 1441 prefunding is acknowledged. This work was supported by the Helmholtz Association Initiative and Networking Fund (grant no. HRSF-0002), the Russian Science Foundation (grant no. 18-41-06001), and the state of Baden-W?rttemberg through bwHPC (bwUniCluster and JUSTUS, RV bw17D011).

Publisher Copyright:
Copyright © 2021 The Authors, some rights reserved.

All Science Journal Classification (ASJC) codes

  • General

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