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Valence Bond Theory02:42

Valence Bond Theory

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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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Ionic crystals consist of two or more different kinds of ions that usually have different sizes. The packing of these ions into a crystal structure is more complex than the packing of metal atoms that are the same size.
Most monatomic ions behave as charged spheres, and their attraction for ions of opposite charge is the same in every direction. Consequently, stable structures for ionic compounds result (1) when ions of one charge are surrounded by as many ions as possible of the opposite...
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Ions are atoms or molecules bearing an electrical charge. A cation (a positive ion) forms when a neutral atom loses one or more electrons from its valence shell, and an anion (a negative ion) forms when a neutral atom gains one or more electrons in its valence shell. Compounds composed of ions are called ionic compounds (or salts), and their constituent ions are held together by ionic bonds: electrostatic forces of attraction between oppositely charged cations and anions. 
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An ionic compound is stable because of the electrostatic attraction between its positive and negative ions. The lattice energy of a compound is a measure of the strength of this attraction. The lattice energy (ΔHlattice) of an ionic compound is defined as the energy required to separate one mole of the solid into its component gaseous ions. For the ionic solid sodium chloride, the lattice energy is the enthalpy change of the process:
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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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超离子旋轮的电离子排序驱动设计

Yubo Wang1, Manas Likhit Holekevi Chandrappa2, Issei Otani3

  • 1Department of Chemistry and the Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo, Ontario N2L3G1, Canada.

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概括

研究人员通过用更便宜的金属取代来开发出具有成本效益的固体电解质用于全固体电池 (ASSB). 这些新材料显示出有前途的离子导电性,为下一代储能铺平了道路.

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科学领域:

  • 材料科学
  • 电化学
  • 计算材料科学

背景情况:

  • 全固态电池 (ASSB) 需要具有成本效益的无机固体电解质 (SE) 来储存下一代能源.
  • 有前途的旋Li2Sc2/3Cl4SE具有高离子导电性,但受到高成本的限制.
  • 开发更低成本的替代品对于ASSB的实际应用至关重要.

研究的目的:

  • 对固体电解质进行选和合成.
  • 研究阴离子替代对离子导电性和稳定性的影响.
  • 建立预测和发现新型固体电解质材料的方法.

主要方法:

  • 结合M3GNET通用机器学习原子间潜力 (UMLIP) 和密度功能理论 (DFT) 进行高效的材料选.
  • 实验合成预测的Mg2+-,Al3+-和Zr4+替代的Li2/Sc2/3/Cl4旋转子.
  • 使用带动力电位 (MTP) 的分子动力学 (MD) 模拟来分析离子传输机制.

主要成果:

  • 合成的Mg2+-,Al3+和Zr4+替代体,其替代分数为20.9%37.5%,其离子导电率高达1.85mS cm-1.
  • 实现了Fe3+的替代,尽管Fe2+的杂质较小.
  • MD模拟显示,Li+/Sc3+/Mn+的排序显著影响了无序的替代组合中的导电性.
  • 具有Li1.75Sc0.416Zr0.25Cl4的证明ASSB在高电流密度 (2mA cm-2) 上运行,具有良好的容量保留 (低速率性能的80%).

结论:

  • 具有成本效益的阴离子替代是一种可行的策略,以减轻基于Sc的体固体电解质的材料成本.
  • 开发的计算方法加速了新型固体电解质的发现.
  • 这项工作为通过合理材料设计设计高性能ASSB提供了基础.