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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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Complexation Equilibria: The Chelate Effect01:19

Complexation Equilibria: The Chelate Effect

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In complexation reactions, metal atoms or cations interact with ligands to form donor-acceptor adducts called metal complexes. Ligands that bind through one donor site are monodentate, ligands with two donor sites are bidentate, and those with more than two donor sites are polydentate ligands. For example, ethylene diamine is a bidentate ligand that binds through two nitrogen donor atoms, forming a five-membered ring. EDTA is a polydentate ligand that binds through four oxygen and two nitrogen...
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Spin–Spin Coupling: Two-Bond Coupling (Geminal Coupling)01:20

Spin–Spin Coupling: Two-Bond Coupling (Geminal Coupling)

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Two NMR-active nuclei bonded to a central atom can be involved in geminal or two-bond coupling. Geminal coupling is commonly seen between diastereotopic protons in chiral molecules and unsymmetrical alkenes, among others.
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The spin state of an NMR-active nucleus can have a slight effect on its immediate electronic environment. This effect propagates through the intervening bonds and affects the electronic environments of NMR-active nuclei up to three bonds away; occasionally, even farther. This phenomenon is called spin–spin coupling or J-coupling. Coupling interactions are mutual and result in small changes in the absorption frequencies of both nuclei involved. While nuclei of the same element are involved...
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Crystal Field Theory
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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Generality Rules and Synergistic Effect of Mitigating the Jahn-Teller Effect by Multisites Compositionally Complex

Shuyu Zhou1,2, Junhong Liao1, Chenglong Yu1

  • 1Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.

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|December 17, 2024
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Multicomponent doping in lithium manganese oxide cathodes suppresses Jahn-Teller distortion, enhancing battery performance. Increasing dopant species reduces structural instability and capacity fading in alkali-ion batteries.

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Jahn−Teller effectcompositionally complex dopinggenerality rulesspinel cathodesynergistic effect

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Jahn-Teller (JT) deformation causes structural distortion and capacity fading in alkali-ion battery cathode materials.
  • Conventional doping strategies have limitations in fully understanding and regulating short-range and cooperative JT effects.

Purpose of the Study:

  • To investigate the impact of multicomponent doping on suppressing Jahn-Teller distortion in spinel LiMn2O4 (LMO) cathodes.
  • To elucidate the relationship between the number of dopant species and the regulation of short-range and cooperative JT effects.

Main Methods:

  • Comparative study of LMO cathodes with varying numbers of dopant species (one, three, five) at tridoping sites.
  • Analysis of MnO6 octahedral distortion, capacity retention, and structural stability.

Main Results:

  • Increasing dopant species systematically decreased MnO6 octahedral distortion and improved capacity retention and structural stability.
  • Mn-site doping disrupted short-range JT distortion, while 16c-site doping mitigated cooperative JT effects by disturbing d-orbital ordering.
  • Complex doping strategy buffered JT strain, leading to isotropic volume distortion and significant suppression of both short-range and cooperative JT effects.

Conclusions:

  • Multicomponent doping offers a synergistic approach to effectively suppress Jahn-Teller distortion in LMO cathodes.
  • The findings provide generality rules for designing high-performance alkali-ion battery cathodes by controlling JT effects through doping strategies.