4.6 Article

A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation

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NATURE CATALYSIS
卷 5, 期 3, 页码 231-237

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NATURE PORTFOLIO
DOI: 10.1038/s41929-022-00756-9

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资金

  1. Australian Research Council Linkage grant [LP150101014, DP190102659, DP200100143, DP210102698, LE200100033]
  2. UNSW Scientia PhD Scholarship Scheme
  3. Microscopy Australia
  4. Mark Wainwright Analytical Centre and Electron Microscope Unit at the University of New South Wales
  5. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy -EXC [2033 390677874 -RESOLV]
  6. US DOE's NNSA [89233218CNA000001]
  7. US DOE's National Nuclear Security Administration [DE-NA-0003525]
  8. Australian Research Council [LE190100021]
  9. US National Science Foundation [OISE-1357113]
  10. US DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
  11. National Key Research and Development Program [2018YFA0208600]
  12. USTC Tang Scholarship
  13. Australian Research Council [LE200100033] Funding Source: Australian Research Council

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Single Pt atom catalysts with high exposure are key targets to enhance electrocatalytic activity, and PtRu alloy nanoparticles are the most active catalysts for the methanol oxidation reaction. This study demonstrates a process to create single-Pt-atom-on-Ru catalysts by growing and spreading Pt islands on Ru branched nanoparticles. The formation of a stable single atom structure is driven by the formation of strong Pt-Ru bonds and the lowering of the surface energy of the Pt islands, resulting in a high current density and mass activity for the methanol oxidation reaction over time.
Single Pt atom catalysts are key targets because a high exposure of Pt substantially enhances electrocatalytic activity. In addition, PtRu alloy nanoparticles are the most active catalysts for the methanol oxidation reaction. To combine the exceptional activity of single Pt atom catalysts with an active Ru support we must overcome the synthetic challenge of forming single Pt atoms on noble metal nanoparticles. Here we demonstrate a process that grows and spreads Pt islands on Ru branched nanoparticles to create single-Pt-atom-on-Ru catalysts. By following the spreading process by in situ TEM, we found that the formation of a stable single atom structure is thermodynamically driven by the formation of strong Pt-Ru bonds and the lowering of the surface energy of the Pt islands. The stability of the single-Pt-atom-on-Ru structure and its resilience to CO poisoning result in a high current density and mass activity for the methanol oxidation reaction over time.

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