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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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Heterogeneous catalysis involves a catalyst in a different phase from the reactants. It is a process where the catalyst and the reactants are in distinct phases, typically solid and gas or liquid.Most heterogeneous catalysts are metals, metal oxides, or acids. The list includes transition metals like iron (Fe), cobalt (Co), nickel (Ni), palladium (Pd), platinum (Pt), chromium (Cr), manganese (Mn), tungsten (W), silver (Ag), and copper (Cu). These metals possess partially vacant d orbitals that...
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Modulating coordinate site occupancy in high-entropy spinel electrocatalysts.

Jihyun Baek1, Kiran Srinivasan Hamkins1,2, Yuzhe Li3

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Controlling cation distribution in high entropy spinel oxides is key for electrocatalysis. Introducing zinc (Zn) into a Co-Fe-Cr-Mn-Ni framework enhances oxygen evolution reaction activity by optimizing cobalt coordination.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • High entropy spinel oxides offer tunable electronic structures for electrocatalysis due to multi-cation incorporation.
  • Controlling cation distribution between tetrahedral and octahedral sites is a significant challenge in designing these catalysts.

Purpose of the Study:

  • To modulate cation coordination site occupancy in a Co-Fe-Cr-Mn-Ni spinel oxide framework.
  • To investigate the effect of introducing a sixth cation (Zn, Ga, Mg, or Al) on cation distribution and electrocatalytic performance.

Main Methods:

  • Density functional theory (DFT) calculations.
  • Synchrotron X-ray absorption spectroscopy (XAS).
  • Magnetic circular dichroism (MCD).

Main Results:

  • Zinc (Zn) preferentially occupies tetrahedral sites, increasing octahedral occupancy of cobalt.
  • This redistribution leads to more octahedrally coordinated cobalt in mixed oxidation states.
  • Enhanced electrical conductivity and improved oxygen evolution reaction (OER) activity were observed.

Conclusions:

  • Coordination site occupancy is a critical design parameter for multicomponent spinel electrocatalysts.
  • Strategic manipulation of cation distribution offers a pathway to optimize catalyst performance.
  • This work provides a rational approach for designing advanced electrocatalysts.