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From Molecules to Materials: Engineering New Ionic Liquid Crystals Through Halogen Bonding
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Exceptionally Bifunctional ORR/OER Performance via Synergistic Atom-Cluster Interaction.

Guanyu Chen1, Yihao Liu1, Shuyan Xue1

  • 1Laboratory of Advanced Materials, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Academy for Engineering & Technology, Fudan University, Shanghai, 200438, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)
|December 10, 2023
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Summary

This study introduces a novel Fe nanocluster and single-atom site catalyst on carbon nanotubes, enhancing oxygen reduction and evolution reactions for efficient Zn-air batteries.

Keywords:
atom–cluster interactionbifunctional electrocatalysiselectron redistribution effectmetal nanocluster

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Single-atom sites (SAs) offer high activity for oxygen reduction reaction (ORR) but suffer from intermediate adsorption and stability issues.
  • Metal clusters provide stability and weak adsorption but lack sufficient active sites for catalysis.

Purpose of the Study:

  • To synthesize and investigate a synergistic framework combining Fe nanoclusters and SAs on 1D carbon nanotubes (Fe3C-NCNTs).
  • To explore the atom-cluster interaction and its impact on electron redistribution and catalytic performance for ORR and oxygen evolution reaction (OER).

Main Methods:

  • Synthesis of Fe nanoclusters combined with SAs on 1D carbon nanotubes (Fe3C-NCNTs).
  • Characterization using off-axis electron holography.
  • Theoretical validation using Density Functional Theory (DFT) calculations.

Main Results:

  • The Fe3C-NCNTs composite demonstrated strong polarization and electron redistribution between nanoclusters and SAs.
  • Electron redistribution enhanced electron transport and intermediate desorption, confirmed by experimental and theoretical analyses.
  • Achieved a 75 mV increase in half-wave potential for ORR and a 133 mV increase for OER compared to catalysts without nanoclusters.
  • Demonstrated high power density and long-term stability in homemade Zn-air batteries (ZABs).

Conclusions:

  • The synergistic Fe nanocluster-SA interaction effectively boosts electrocatalytic activity for both ORR and OER.
  • This approach provides a facile route for designing bifunctional electrocatalysts for energy storage applications like ZABs.
  • The developed 0D composite structure offers a promising strategy for advanced catalyst design.