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Second-Shell N Dopants Regulate Acidic O2 Reduction Pathways on Isolated Pt Sites.

Baoxin Ni1,2, Peng Shen2, Guiru Zhang2

  • 1National Key Laboratory of Advanced Micro and Nano Manufacture Technology, Department of Micro/Nano Electronics, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.

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Nitrogen dopants in platinum-nitrogen-carbon single-atom catalysts precisely control the oxygen reduction reaction (ORR) pathway. This research tailors selectivity for efficient energy conversion, crucial for fuel cells.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Platinum (Pt) is a benchmark catalyst for the acidic oxygen reduction reaction (ORR), essential for energy conversion.
  • Controlling the ORR pathway in single-atom catalysts (SACs) is challenging due to complex coordination environments.

Purpose of the Study:

  • To investigate how neighboring nitrogen (N) dopants influence the electronic structure of Pt single atoms.
  • To demonstrate the tuning of ORR selectivity (O2-to-H2O vs. O2-to-H2O2) in Pt-N-C SACs.

Main Methods:

  • Synthesis of carbon nanotube supported Pt-N-C single-atom catalysts.
  • Utilized X-ray-radiated spectroscopy and shell-isolated nanoparticle-enhanced Raman spectroscopy.
  • Employed theoretical modeling for comprehensive analysis.

Main Results:

  • Achieved tunable O2-to-H2O2 selectivity from 10% to 85% at 0.3 V by altering N dopant coordination.
  • Pyridinic- and pyrrolic-N coordination favored the 4-electron ORR pathway.
  • Second-shell graphitic-N introduction weakened *OOH binding, promoting the 2-electron ORR pathway.

Conclusions:

  • The local chemical environment, specifically N dopant coordination, is critical for steering ORR selectivity in Pt SACs.
  • Demonstrated a strategy to precisely control electrochemical performance by manipulating the coordination sphere of single-atom catalysts.