Abstract
We herein present a study on the sodiation/desodiation behavior of Na3V2(PO4)2O1.6F1.4 cathode with I4/mmm tetragonal space group by the combination of dual-mode electron paramagnetic resonance (EPR) and in situ/ex situ solid-state nuclear magnetic resonance (SSNMR) techniques. The complementary parallel/perpendicular mode EPR, in situ 23Na NMR, 23Na/51V MAS NMR, and two-dimensional 23Na MQMAS NMR experiments substantiate that (i) both VIV and VIII are electrochemically active in this material, with the former transforming to VV, whereas the latter transforming to VIV; (ii) VIV continually converts to VV during the whole charge process, whereas VIII mostly reacts at the higher-potential charge plateau region; (iii) the Na+ extraction/intercalation process of Na3V2(PO4)2O1.6F1.4 is a widespread solid-solution mechanism; (iv) electronic spin hopping might occur locally between VIII and VV ions generated during the electrochemical reaction, resulting in the inconsecutive shift in 23Na resonance. This study s...
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