Local and Bulk Probe of Vanadium-Substituted α-Manganese Oxide (α-KxVyMn8–yO16) Lithium Electrochemistry

Lutz, Diana M.; Dunkin, Mikaela R.; Tallman, Killian R.; Wang, Lei; Housel, Lisa M.; Yang, Shize; Zhang, Bingjie; Liu, Ping; Bock, David C.; Zhu, Yimei; Marschilok, Amy C.; Takeuchi, Esther S.; Takeuchi, Kenneth J.

doi:10.1021/acs.inorgchem.1c00954

Title: Local and Bulk Probe of Vanadium-Substituted α-Manganese Oxide (α-K_xV_yMn_8–yO₁₆) Lithium Electrochemistry

Journal Article · Thu Jul 08 00:00:00 EDT 2021 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.1c00954· OSTI ID:1822337

^[1]; Dunkin, Mikaela R. ^[1]; Tallman, Killian R. ^[1];

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^[2]; Yang, Shize ^[3]; Zhang, Bingjie ^[4];

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Stony Brook Univ., NY (United States); Stony Brook Univ., NY (United States). Inst. for Electrochemically Stored Energy
Stony Brook Univ., NY (United States). Inst. for Electrochemically Stored Energy; Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Department of Chemistry, Stony Brook University, Stony Brook, New York 11794, United States
Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States). Inst. for Electrochemically Stored Energy; Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

A series of V-substituted α-MnO₂ (K_{_x}Mn_{_8–y}V_{_y}O_₁₆·nH₂O, y = 0, 0.2, 0.34, 0.75) samples were successfully synthesized without crystalline or amorphous impurities, as evidenced by X-ray diffraction (XRD) and Raman spectroscopy. Furthermore, transmission electron microscopy (TEM) revealed a morphological evolution from nanorods to nanoplatelets as V-substitution increased, while electron-energy loss spectroscopy (EELS) confirmed uniform distribution of vanadium within the materials. Rietveld refinement of synchrotron XRD showed an increase in bond lengths and a larger range of bond angles with increasing V-substitution. X-ray absorption spectroscopy (XAS) of the as-prepared materials revealed the V valence to be >4+ and the Mn valence to decrease with increasing V content. Upon electrochemical lithiation, increasing amounts of V were found to preserve the Mn–Mn_edge relationship at higher depths of discharge, indicating enhanced structural stability. Electrochemical testing showed the y = 0.75 V-substituted sample to deliver the highest capacity and capacity retention after 50 cycles. The experimental findings were consistent with the predictions of density functional theory (DFT), where the V centers impart structural stability to the manganese oxide framework upon lithiation. The enhanced electrochemistry of the y = 0.75 V-substituted sample is also attributed to its smaller crystallite size in the form of a nanoplatelet morphology, which promotes facile ion access via reduced Li-ion diffusion path lengths.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; SC0012673; 1839287

OSTI ID:: 1822337

Report Number(s):: BNL-222173-2021-JAAM; TRN: US2214457

Journal Information:: Inorganic Chemistry, Vol. 60, Issue 14; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Morphology
Vanadium
Transition metals
Diffraction
Materials

Title: Local and Bulk Probe of Vanadium-Substituted α-Manganese Oxide (α-KxVyMn8–yO16) Lithium Electrochemistry

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Title: Local and Bulk Probe of Vanadium-Substituted α-Manganese Oxide (α-K_xV_yMn_8–yO₁₆) Lithium Electrochemistry