Elucidating the Impact of Mg Substitution on the Properties of NASICON-Na_(3+y)V_(2-y)Mg_y(PO_4)_3 Cathodes

Ghosh Subham; Barman Nabadyuti; Gonzalez-Correa EliovardoMazumder MadhulikaZaveri AryanGiovine RaynaldManche AlexisPati Swapan K.Clement Raphaele J.Senguttuvan Premkumar

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Elucidating the Impact of Mg Substitution on the Properties of NASICON-Na_(3+y)V_(2-y)Mg_y(PO_4)_3 Cathodes

机译：Elucidating the Impact of Mg Substitution on the Properties of NASICON-Na_(3+y)V_(2-y)Mg_y(PO_4)_3 Cathodes

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Vanadium multiredox-based NASICON-NazV2-yMy(PO4)(3) (3 = z = 4; M = Al3+, Cr3+, and Mn2+) 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 (approximate to 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 Mg2+-substituted Na3+yV2-yMgy(PO4)(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 Mg2+ substitution for V3+. Concurrently, the intercalation voltage rises from 3.35 to 3.45 V, due to increasingly more ionic V-O 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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《Advanced functional materials》 |2021年第48期|2105463.1-2105463.11|共11页
作者
Ghosh Subham; Barman Nabadyuti; Gonzalez-Correa EliovardoMazumder MadhulikaZaveri AryanGiovine RaynaldManche AlexisPati Swapan K.Clement Raphaele J.Senguttuvan Premkumar;
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Jawaharlal Nehru Ctr Adv Sci Res, New Chem Unit, Bangalore 560064, Karnataka, India|Jawaharlal Nehru Ctr Adv Sci Res, Int Ctr Mat Sci, Bangalore 560064, Karnataka, India|Jawaharlal Nehru Ctr Adv Sci Res, Sch Adv Mat, Bangalore 560064, Karnataka, India;

Univ Calif Santa Barbara, Mat Dept, Santa Barbara, CA 93106 USA|Univ Calif Santa Barbara, Mat Res Lab, Santa Barbara, CA 93106 USA;

Jawaharlal Nehru Ctr Adv Sci Res, New Chem Unit, Bangalore 560064, Karnataka, India|Jawaharlal Nehru Ctr Adv Sci Res, Sch Adv Mat, Bangalore 560064, Karnataka, India|Jawaharlal Nehru Ctr Adv Sci Res, Theoret Sci Unit, Bangalore 560064, Karnataka, IndiaUniv Calif Santa Barbara, Mat Res Lab, Santa Barbara, CA 93106 USA|Univ Calif Santa Barbara, Phys Dept, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Mat Dept, Santa Barbara, CA 93106 USA|Univ Bordeaux, UF Chim, F-33405 Talence, France|Univ St Andrews, Sch Chem, St Andrews KY16 9ST, Fife, ScotlandJawaharlal Nehru Ctr Adv Sci Res, Sch Adv Mat, Bangalore 560064, Karnataka, India|Jawaharlal Nehru Ctr Adv Sci Res, Theoret Sci Unit, Bangalore 560064, Karnataka, India;

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Mg substitution; NASICON cathodes; sodium-ion batteries;

Elucidating the Impact of Mg Substitution on the Properties of NASICON-Na_(3+y)V_(2-y)Mg_y(PO_4)_3 Cathodes

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