4.8 Article

Three-Dimensional Tracking and Visualization of Hundreds of Pt-Co Fuel Cell Nanocatalysts During Electrochemical Aging

Journal

NANO LETTERS
Volume 12, Issue 9, Pages 4417-4423

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/nl203920s

Keywords

Tomography; electrocatalysis; STEM; fuel cell; ORR; EELS

Funding

  1. Center for Nanoscale Systems
  2. NDSEG fellowship
  3. Department of Energy [DE-FG02-87ER45298]
  4. Energy Materials Center at Cornell, an Energy Frontier Research Center
  5. U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0001086]
  6. National Science Foundation Materials Research Science and Engineering Centers (MRSEC) program [DMR 1120296]
  7. U.S. Department of Energy (DOE) [DE-FG02-87ER45298] Funding Source: U.S. Department of Energy (DOE)

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We present an electron tomography method that allows for the identification of hundreds of electrocatalyst nanoparticles with one-to-one correspondence before and after electrochemical aging. This method allows us to track, in three-dimensions, the trajectories and morphologies of each Pt-Co nanocatalyst on a fuel cell carbon support. In conjunction with the use of atomic-scale electron energy loss spectroscopic imaging, our experiment enables the correlation of performance degradation of the catalyst with changes in particle/interparticle morphologies, particle-support interactions, and the near-surface chemical composition. We found that aging of the catalysts under normal fuel cell operating conditions (potential scans from +0.6 to +1.0 V for 30 000 cycles) gives rise to coarsening of the nanoparticles, mainly through coalescence, which in turn leads to the loss of performance. The observed coalescence events were found to be the result of nanoparticle migration on the carbon support during potential cycling. This method provides detailed insights into how nanocatalyst degradation occurs in proton exchange membrane fuel cells (PEMFCs) and suggests that minimization of particle movement can potentially slow down the coarsening of the particles and the corresponding performance degradation.

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