Insight into the Fast-Rechargeability of a Novel Mo1.5W1.5Nb14O44 Anode Material for High-Performance Lithium-Ion Batteries
ADVANCED ENERGY MATERIALS(2022)
摘要
Wadsley-Roth phased niobates are promising anode materials for lithium-ion batteries, while their inherently low electrical conductivity still limits their rate-capability. Herein, a novel doped Mo1.5W1.5Nb14O44 (MWNO) material is facilely prepared via an ionothermal-synthesis-assisted doping strategy. The detailed crystal structure of MWNO is characterized by neutron powder diffraction and aberration corrected scanning transmission electron microscope, unveiling the full occupation of Mo6+-dopant at the t1 tetrahedral site. In half-cells, MWNO exhibits enhanced fast-rechargeability. The origin of the improved performance is investigated by ultraviolet-visible diffuse reflectance spectroscopy, density functional theory (DFT) computation, and electrochemical impedance spectroscopy, revealing that bandgap narrowing improves the electrical conductivity of MWNO. Furthermore, operando X-ray diffraction elucidates that MWNO exhibits a typical solid-solution phase conversion-based lithium-ion insertion/extraction mechanism with reversible structural evolution during the electrochemical reaction. The boosted lithium-ion diffusivity of MWNO, due to the Mo6+/W6+ doping effect, is confirmed by a galvanostatic intermittent titration technique and DFT. With the simultaneously enhanced electrical conductivity and lithium-ion diffusivity, MWNO successfully demonstrates its fast-rechargeability and practicality in the LiNi0.5Mn1.5O4-coupled full-cells. Therefore, this work illustrates the potential of ionothermal synthesis in energy storage materials and provides a mechanistic understanding of the doping effect on improving material's electrochemical performance.
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关键词
doping, electrical conductivity, fast-rechargeable lithium-ion batteries, ionothermal synthesis, lithium-ion diffusivity, Mo1 5W1 5Nb14O44
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