To provide bioelectrets with controlled electrical energy, the polarization and relaxation characteristics of hydroxyapatite (HA) ceramic electrets were investigated in terms of poling conditions and microstructures. HA electrets were prepared between 250 and 500 °C for 5–120 min under a 5 kV cm−1 dc electrical field. Poling conditions and grain size of HA ceramics significantly influenced the thermally stimulated depolarization current (TSDC) spectra and charge storage (Q). Under a poling field of 5 kV cm−1, varying the poling temperature from 250 to 500 °C drastically shifted the TSDC peak temperature from 250 to 620 °C and increased Q from 0.5 to 45 μC cm−2. The change in the average grain size from 2 to 11 μm increased the Q value from 15 to 60 μC cm−2 with a negligible shift in the TSDC peak position. The measured difference of the TSDC peak shapes and positions, as well as the Q values, was theoretically due to the four polarization states with different activation energies (Edr) of dipole relaxation and the pre-exponential factor of relaxation times (τ0). The dependences on the poling conditions and grain size indicated that the four states were due to the orientation polarization of absorbed water (state 1), the localizations of displaced protons around PO43− and OH− in the grains (states 2 and 3), and the localization of displaced protons in the grain boundaries (state 4).
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