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Nano Si-Doped Ruthenium Oxide Particles from Caged Precursors for High-Performance Acidic Oxygen Evolution.

Chunxiang Liu1, Yunbo Jiang2, Teng Wang1,3

  • 1School of Chemistry, Beihang University, Beijing, 100191, P. R. China.

Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|February 22, 2023
PubMed
Summary

Ruthenium oxide (RuO2) durability for the oxygen evolution reaction (OER) is enhanced by trapping precursors in a cage compound. This creates stable, highly active Si-RuOx@C catalysts for acidic conditions.

Keywords:
caged precursorsoxygen evolution reactionruthenium oxide particles

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Ruthenium dioxide (RuO2) is a benchmark catalyst for the acidic oxygen evolution reaction (OER).
  • Limited durability of RuO2 hinders its practical application in OER catalysis.
  • Developing stable and efficient OER catalysts is crucial for energy conversion technologies.

Purpose of the Study:

  • To enhance the stability and activity of ruthenium oxide catalysts for acidic OER.
  • To investigate the effect of precursor organization on catalyst performance.
  • To explore the role of silicon doping in improving catalyst durability and efficiency.

Main Methods:

  • Pre-trapping of RuCl3 precursors within a 72-aromatic-ring cage compound.
  • Calcination to form well carbon-coated RuOx particles (Si-RuOx@C).
  • Electrochemical testing in 0.5 M H2SO4 at 10 mA cm-2.
  • X-ray absorption fine structure (FT-EXAFS) and density functional theory (DFT) calculations.

Main Results:

  • The Si-RuOx@C catalyst demonstrated unprecedented stability, operating for 100 hours with minimal overpotential change.
  • The catalyst exhibited a low overpotential of 220 mV at 10 mA cm-2 in acidic solution.
  • FT-EXAFS confirmed Si doping via a unique Ru-Si bond.
  • DFT calculations highlighted the critical role of the Ru-Si bond in enhancing catalyst activity and stability.

Conclusions:

  • Pre-organization of Ru precursors within a cage structure significantly improves the durability of RuOx catalysts.
  • The novel Si-RuOx@C catalyst offers superior performance and stability for acidic OER compared to commercial RuO2.
  • The identified Ru-Si bond is key to the enhanced catalytic properties, paving the way for advanced OER catalyst design.