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Valence Bond Theory02:42

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Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
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Engineering Spin-Electronic Coupling at Fe Cluster/Single-Atom Interfaces via p-Block Modulation for Zn-Air

Lulu Lyu1, Wenqi Fan1, Xu Hu2

  • 1Department of Materials Science and Engineering, Korea University, Seoul, Republic of Korea.

Advanced Materials (Deerfield Beach, Fla.)
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Summary
This summary is machine-generated.

This study introduces a new Fe-N-C catalyst with Sb for zinc-air batteries (ZABs). The catalyst enhances oxygen reduction reaction (ORR) kinetics, leading to improved battery performance and durability, even at low temperatures.

Keywords:
5p–3d hybridizationAh‐level Zn‐air batteryFe cluster/SACdual electronic–spin modulationoxygen reduction reaction

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Area of Science:

  • Electrochemistry and Materials Science
  • Catalysis for Energy Storage

Background:

  • Iron-nitrogen-carbon (Fe-N-C) single-atom catalysts are promising for zinc-air batteries (ZABs).
  • Oxygen reduction reaction (ORR) kinetics are limited by strong intermediate binding at FeN4 sites.

Purpose of the Study:

  • To develop a novel heterostructured catalyst to overcome kinetic limitations in ZABs.
  • To improve the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity.

Main Methods:

  • Fabrication of a heterostructured catalyst (FeAC/SbFeNC) with sub-nanometer Fe clusters coupled to Sb and Fe sites on N-doped carbon.
  • Utilized operando spectroscopic analyses and first-principles calculations.
  • Tested catalyst performance in aqueous and quasi-solid-state ZABs.

Main Results:

  • Sb acts as an electronic modulator, redistributing charge and quenching magnetic moments via 5p-3d hybridization.
  • Coupled electronic-spin modulation significantly lowers ORR energy barriers for O-O bond cleavage and *OH desorption.
  • Achieved a peak power density of 244.6 mW cm⁻² and 2300 h lifespan in aqueous ZABs.
  • Demonstrated excellent performance in quasi-solid-state ZABs, including 1.12 Ah capacity and 600 h operation at -40°C.

Conclusions:

  • The FeAC/SbFeNC catalyst exhibits enhanced bifunctional activity for ZABs.
  • Synergistic interplay between p-block electronic/spin modulation and metal clusters is an effective strategy to overcome ORR limitations.
  • This approach offers a pathway for developing high-performance, durable ZABs for demanding applications.