Structure, Defect Chemistry,
and Lithium Transport
Pathway of Lithium Transition Metal Pyrophosphates (Li<sub>2</sub>MP<sub>2</sub>O<sub>7</sub>, M: Mn, Fe, and Co): Atomistic Simulation
Study
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Abstract
Lithium transition metal pyrophosphate materials (Li<sub>2</sub>MP<sub>2</sub>O<sub>7</sub>, M: Mn, Fe, and Co) have been
proposed
as promising novel cathode materials for lithium ion batteries. Using
atomistic simulation with empirical potential parameters, which has
been validated on various cathode materials by Islam et al. [<i>Phil. Trans. R. Soc. A</i> <b>2010</b>, <i>368</i>, 3255–3267], these new pyrophosphates are investigated to
elucidate structure, defect chemistry, and Li<sup>+</sup> ion transport
pathway. The core–shell model with empirical force fields reproduces
the experimental unit-cell parameters, and formation energies of intrinsic
defects (Frenkel and antisite) are calculated. From migration energy
calculation, it is found that the pyrophosphates without partial occupation
have a 2D Li<sup>+</sup> ion pathway. Meanwhile, under the condition
of partial occupancies of Li and transition metal atoms, the diffusion
pathway of Li<sup>+</sup> ions is a 3D network