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The alkali metal sodium (atomic number 11) has one more electron than the neon atom. This electron must go into the lowest-energy subshell available, the 3s orbital, giving a 1s22s22p63s1 configuration. The electrons occupying the outermost shell orbital(s) (highest value of n) are called valence electrons, and those occupying the inner shell orbitals are called core electrons. Since the core electron shells correspond to noble gas electron configurations, we can abbreviate electron...
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To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
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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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Tetrahedral Complexes
Crystal field theory (CFT) is applicable to molecules in geometries other than octahedral. In octahedral complexes, the lobes of the dx2−y2 and dz2 orbitals point directly at the ligands. For tetrahedral complexes, the d orbitals remain in place, but with only four ligands located between the axes. None of the orbitals points directly at the tetrahedral ligands. However, the dx2−y2 and dz2 orbitals (along the Cartesian axes) overlap with the ligands less than the dxy,...
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Alkenes are converted to 1,2-diols or glycols through a process called dihydroxylation. It involves the addition of two hydroxyl groups across the double bond with two different stereochemical approaches, namely anti and syn. Dihydroxylation using osmium tetroxide progresses with syn stereochemistry.
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Heteroatom-Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction.

Leilei Yin1, Shuai Zhang1, Mingzi Sun2

  • 1Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, Haihe Laboratory of Sustainable Chemical Transformations, Smart Sensing Interdisciplinary Science Center, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin, 300350, China.

Advanced Materials (Deerfield Beach, Fla.)
|April 4, 2023
PubMed
Summary

This study introduces novel cerium single-atom catalysts (Ce SAs) on a doped carbon support for enhanced oxygen reduction reactions (ORR). These catalysts show superior performance in zinc-air batteries and flexible devices.

Keywords:
coordination modulationheteroatom dopingoxygen reduction reactionrare-earth elementssingle-atom catalyst

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Modulating rare-earth single-atom catalysts (SACs) with complex electronic structures remains a challenge.
  • Developing efficient catalysts for oxygen reduction reactions (ORR) is crucial for energy conversion and storage.

Purpose of the Study:

  • To synthesize and characterize cerium single atoms (Ce SAs) supported on a P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC).
  • To evaluate the electrocatalytic performance of Ce SAs/PSNC for the oxygen reduction reaction (ORR).
  • To investigate the application of Ce SAs/PSNC in liquid zinc-air batteries (ZABs) and flexible electronic devices.

Main Methods:

  • Synthesis of P, S, and N co-doped hollow carbon substrate.
  • Immobilization of cerium single atoms onto the carbon substrate.
  • Electrochemical characterization including half-wave potential and turnover frequency measurements.
  • Fabrication and testing of liquid zinc-air batteries.
  • Density functional theory (DFT) calculations to understand electronic modulations.

Main Results:

  • Ce SAs/PSNC exhibited a high half-wave potential of 0.90 V and a turnover frequency of 52.2 s-1 at 0.85 V for ORR.
  • The catalyst demonstrated excellent stability, outperforming commercial Pt/C and other SACs.
  • Ce SAs/PSNC-based ZABs achieved a high open-circuit voltage of 1.49 V and a power density of 212 mW cm-2.
  • Theoretical calculations confirmed that P and S doping significantly modulated the electronic structure of Ce SAs, enhancing electroactivity and electron transfer.

Conclusions:

  • The P, S, and N co-doped hollow carbon substrate effectively modulates the coordination environment of Ce single atoms.
  • Ce SAs/PSNC is a highly efficient and stable catalyst for ORR, suitable for ZABs and flexible devices.
  • This work provides a new strategy for designing rare-earth-based SACs for advanced energy applications.