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For transition metal complexes, the coordination number determines the geometry around the central metal ion. Table 1 compares coordination numbers to molecular geometry. The most common structures of the complexes in coordination compounds are octahedral, tetrahedral, and square planar.
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Energy production within a cell involves many coordinated chemical pathways. Most of these pathways are combinations of oxidation and reduction reactions, which occur at the same time. An oxidation reaction strips an electron from an atom in a compound, and the addition of this electron to another compound is a reduction reaction. Because oxidation and reduction usually occur together, these pairs of reactions are called redox reactions.
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Tuning the Acidity of Pt/ CNTs Catalysts for Hydrodeoxygenation of Diphenyl Ether
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Coordination Tunes Selectivity: Two-Electron Oxygen Reduction on High-Loading Molybdenum Single-Atom Catalysts.

Cheng Tang1, Yan Jiao1, Bingyang Shi2

  • 1Centre for Materials in Energy and Catalysis, School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia.

Angewandte Chemie (International Ed. in English)
|March 21, 2020
PubMed
Summary

This study introduces novel Molybdenum single-atom catalysts (SACs) with unique O,S coordination for efficient electrocatalysis. These advanced SACs demonstrate high selectivity for hydrogen peroxide production via the oxygen reduction reaction.

Keywords:
electrocatalysismolybdenumoxygen reduction reaction (ORR)selectivitysingle-atom catalyst

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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Single-atom catalysts (SACs) offer high efficiency in electrocatalysis but face challenges in synthesis and understanding structure-property relationships.
  • Optimizing SAC performance requires careful control over metal atoms, dopants, and loading, which is synthetically demanding.

Purpose of the Study:

  • To develop a novel Molybdenum-based single-atom catalyst (Mo SAC) with a unique oxygen-sulfur (O,S) coordination and high metal loading.
  • To investigate the structure-property relationships governing the catalytic activity of the developed Mo SACs.

Main Methods:

  • Synthesis of Mo SACs with high metal loading (>10 wt%).
  • Characterization using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and extended X-ray absorption fine structure (EXAFS) to identify atomic isolation and local coordination.
  • Electrochemical testing to evaluate catalytic performance for the oxygen reduction reaction (ORR).
  • Theoretical calculations to elucidate the catalytic mechanism and the role of single atoms and coordination structure.

Main Results:

  • A novel Mo SAC featuring a unique O,S coordination environment and high metal loading (>10 wt%) was successfully synthesized.
  • The Mo SAC demonstrated high selectivity (>95%) for producing hydrogen peroxide (H$_{2}$O$_{2}$) via a 2-electron pathway in the oxygen reduction reaction (ORR) in 0.10 M KOH.
  • Atomic-level characterization confirmed the presence and local environment of isolated Mo single atoms.

Conclusions:

  • The developed Mo SAC with O,S coordination exhibits excellent performance for the 2-electron ORR, selectively producing H$_{2}$O$_{2}$.
  • The study highlights the critical role of isolated Mo single atoms and their specific coordination structure in achieving high catalytic selectivity.
  • This work provides insights into rational design strategies for advanced single-atom catalysts in electrocatalysis.