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000474147 1001_ $$0P:(DE-H253)PIP1081280$$aGhosh, Subham$$b0
000474147 245__ $$aElucidating the Impact of Mg Substitution on the Properties of NASICON‐Na$_{3+y}$V$_{ 2−y}$Mg$_y$(PO$_4$)$_ 3$ Cathodes
000474147 260__ $$aWeinheim$$bWiley-VCH$$c2021
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000474147 500__ $$aThe  authors  acknowledge  DESY  (Hamburg,  Germany),  a  member  of  the  Helmholtz  Association  HGF,  for  the  provision  of  experimental  facilities.  Parts  of  this  research  were  carried  out  at  PETRA  III  and  the  authors  thank  Dr.  Edmund  Welter  for  his  assistance  in  using  Beamline  P65,  and  DST  for  financial  assistance  for  the  measurement  at  DESY.
000474147 520__ $$aVanadium multiredox-based NASICON-NazV2−yMy(PO$_4$)$_3$ (3 ≤ z ≤ 4; M = Al$^{3+}$, Cr$^{3+}$, and Mn$^{2+}$) cathodes are particularly attractive for Na-ion battery applications due to their high Na insertion voltage (>3.5 V vs Na$^+$/Na$^0$), reversible storage capacity (≈150 mA h g$^{-1}$), and rate performance. However, their practical application is hindered by rapid capacity fade due to bulk structural rearrangements at high potentials involving complex redox and local structural changes. To decouple these factors, a series of Mg$^{2+}$-substituted Na$_{3+y}$V$_{ 2−y}$Mg$_y$(PO$_4$)$_ 3$ (0 ≤ y ≤ 1) cathodes is studied for which the only redox-active species is vanadium. While X-ray diffraction (XRD) confirms the formation of solid solutions between the y = 0 and 1 end members, X-ray absorption spectroscopy and solid-state nuclear magnetic resonance reveal a complex evolution of the local structure upon progressive Mg$^{2+}$ substitution for V$^{3+}$. Concurrently, the intercalation voltage rises from 3.35 to 3.45 V, due to increasingly more ionic VO bonds, and the sodium (de)intercalation mechanism transitions from a two-phase for y ≤ 0.5 to a solid solution process for y ≥ 0.5, as confirmed by in operando XRD, while Na-ion diffusion kinetics follow a nonlinear trend across the compositional series.
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000474147 7001_ $$0P:(DE-H253)PIP1082593$$aBarman, Nabadyuti$$b1
000474147 7001_ $$aGonzalez-Correa, Eliovardo$$b2
000474147 7001_ $$aMazumder, Madhulika$$b3
000474147 7001_ $$aZaveri, Aryan$$b4
000474147 7001_ $$aGiovine, Raynald$$b5
000474147 7001_ $$aManche, Alexis$$b6
000474147 7001_ $$aPati, Swapan K.$$b7
000474147 7001_ $$aClément, Raphaële J.$$b8
000474147 7001_ $$0P:(DE-H253)PIP1033129$$aSenguttuvan, Premkumar$$b9$$eCorresponding author
000474147 773__ $$0PERI:(DE-600)2039420-2$$a10.1002/adfm.202105463$$gVol. 31, no. 48, p. 2105463 -$$n48$$p2105463$$tAdvanced functional materials$$v31$$x1057-9257$$y2021
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