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Constructing artificial interphase layer of polyoxovanadates with high oxidizability and reversibility to boost dendrite-free lithium metal anode

Song, Y.; Zhang, J.; Zhang, C.; Fan, L.; Song, J.; Cao, Y.; Feng, Y.; Liu, H.; Gao, G.

Chemical Engineering Journal 519: 165237

2025

ISSN/ISBN: 1385-8947
DOI: 10.1016/j.cej.2025.165237
Accession: 095113352

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Summary
This study selects three polyoxovanadates (POVs) (Na6[VV10O28]·18H2O, V10; Li7[VIV8VV7O36(CO3)]·nH2O, V15; K10[VIV16VV18O82]·20H2O, V34) to chemically modify lithium metal anode, with the aim of constructing an artificial interphase layer to modulate deposition behavior of lithium. By comparing effects of these POVs, V34 with higher oxidizability facilitates the formation of a dense and robust safeguarding stratum on lithium surface, which homogenizes distribution of Li+ flux and efficiently suppresses side reactions between lithium metal and electrolyte. Theoretical calculations indicate that lithium tends to be adsorbed at structural neck of V34, which suggests its effectiveness in directionally regulating lithium deposition and reducing diffusion energy barrier of Li+. More significantly, V34 exhibits high redox activity and excellent redox reversibility compared with V10 and V15, enabling it to function as an "ion sponge" that repeatedly binds to and dissociates from lithium during stripping/plating processes. The symmetrical cell with V34 modified lithium foil delivers exceptional cyclic stability for 1350 cycles at 3 mA cm−2 and 1 mAh cm−2. The Li[sbnd]S cell shows superior discharge capacity of 418.1 mAh g−1 at 1C after 200 cycles, and it achieves a reversible capacity of 490.8 mAh g−1 after 100 cycles at 0.2C under sulfur loading of ∼4.0 mg cm−2.

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