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Ion coordination and migration mechanisms in alkali metal complex borohydride-based solid electrolytes.

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Non-covalent dispersion interactions in solid electrolytes (SEs) regulate ion migration. These interactions, specifically many-body dispersion (MBD) interactions, influence ion diffusion barriers and lead to anomalous diffusion in M2B12H12 frameworks.

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Area of Science:

  • Materials Science
  • Solid-state Chemistry
  • Computational Chemistry

Background:

  • Solid electrolytes (SEs) utilize static anion frameworks and mobile cation sublattices.
  • Non-covalent dispersion interactions (Edisp) are crucial for SE structural stability.
  • The precise role of Edisp in cation (M-ion) migration within SEs is not fully understood.

Purpose of the Study:

  • To investigate M-ion diffusion barriers in M2B12H12 solid electrolytes.
  • To elucidate the specific role of non-covalent interactions in M-ion migration.
  • To understand the impact of different alkali ions (Li, Na, K) on these interactions and diffusion.

Main Methods:

  • Computational analysis of M2B12H12 (M = Li, Na, K) solid electrolytes.
  • Examination of many-body dispersion (MBD) interactions and their influence on cation mobility.
  • Correlation analysis between effective coordination number (ECN) and dispersion interactions (Edisp).

Main Results:

  • Significant changes in MBD interactions were observed across Li, Na, and K analogues.
  • MBD interactions function as 'springs' within the framework, regulating the effective coordination number (ECN) of M-ions.
  • A linear correlation between ECN and Edisp was identified, revealing a unified mechanism for M-ion migration regulation.
  • Dispersion interactions were found to influence the prefactor in the diffusivity equation, leading to anomalous diffusion.

Conclusions:

  • Dispersion interactions are key to regulating M-ion migration barriers in M2B12H12 SEs.
  • A critical bottleneck for diffusion of ions heavier than lithium was identified in these SEs.
  • Many-body dispersion interactions significantly impact ion diffusion dynamics and can drive anomalous diffusion behavior.