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In-Situ Generated High-Valent Iron Single-Atom Catalyst for Efficient Oxygen Evolution.

Zhirong Zhang1, Chen Feng1, Xiangyang Li1

  • 1Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, National Synchrotron Radiation Laboratory, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.

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|May 21, 2021
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Summary

A novel single-atom iron catalyst with Fe⁴⁺ centers shows high activity for the oxygen evolution reaction (OER), a key process in renewable energy. This iron-based catalyst offers a promising, efficient alternative for electrochemical applications.

Keywords:
high-valent ironoxygen evolutionsingle atom catalysts

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Oxygen evolution reaction (OER) is crucial for renewable energy and chemical transformations.
  • Iron-based catalysts are abundant but typically show limited activity for OER.

Purpose of the Study:

  • To develop a highly active iron-based catalyst for OER.
  • To investigate the mechanism behind the enhanced catalytic activity.

Main Methods:

  • Synthesis of a single-atom iron catalyst supported on carbon.
  • Electrochemical characterization of the catalyst's OER performance.
  • In-situ generation of Fe⁴⁺ active sites.
  • Theoretical calculations (DFT) to understand reaction mechanisms.

Main Results:

  • The single-atom iron catalyst achieved 10 mA cm⁻² at an overpotential of 320 mV.
  • An ultrahigh turnover frequency of 0.62 s⁻¹ at 0.35 V was observed.
  • Experimental and theoretical studies confirmed the in-situ generation of highly active Fe⁴⁺ species.
  • Strong Fe-C interaction via C-O-Fe bonding facilitated OER by lowering the *OOH formation barrier.

Conclusions:

  • Single-atom iron catalysts with in-situ generated Fe⁴⁺ centers exhibit exceptional OER activity.
  • The unique Fe-C bonding is key to the catalyst's performance.
  • This work presents a promising strategy for designing efficient earth-abundant OER catalysts.