Semi-Ionic F Modified N-Doped Porous Carbon Implanted with Ruthenium Nanoclusters toward Highly Efficient...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Developing efficient electrocatalysts for the hydrogen evolution reaction (HER) across all pH levels remains a significant challenge.
• Ruthenium (Ru)-based catalysts often suffer from strong intermediate binding and slow water dissociation, limiting their activity.
• Designing catalysts with tunable electronic properties and optimized active sites is crucial for advancing HER.

Purpose of the Study:

• To develop a novel ruthenium-based electrocatalyst with enhanced pH-universal hydrogen evolution reaction (HER) activity and durability.
• To investigate the synergistic effects between ruthenium nanoclusters and a modified porous carbon support.
• To elucidate the mechanism behind the improved catalytic performance using theoretical calculations.

Main Methods:

• A hydrogel sealing-pyrolysis-etching strategy was employed to synthesize F-modified N-doped porous carbon implanted with ruthenium nanoclusters (Ru/FNPC).
• Electrochemical performance was evaluated through hydrogen evolution reaction (HER) measurements in alkaline, neutral, and acidic media.
• Density functional theory (DFT) calculations were performed to understand the electronic structure and reaction mechanisms.

Main Results:

• The optimal 8Ru/FNPC catalyst exhibited ultralow overpotentials of 17.8 mV (alkaline), 71.2 mV (neutral), and 53.8 mV (acidic) at 10 mA cm⁻².
• The catalyst demonstrated exceptional HER reactivity and stability across the entire pH range.
• DFT calculations confirmed that F-doping weakens intermediate adsorption and lowers energy barriers for HER.

Conclusions:

• The synthesized Ru/FNPC catalyst shows remarkable potential for highly efficient and pH-universal hydrogen generation.
• The synergistic interaction between Ru nanoclusters and the F, N-codoped porous carbon support is key to the enhanced performance.
• This study offers valuable insights into designing advanced electrocatalysts for energy conversion applications.