Insight into the Fast-Rechargeability of a Novel Mo1.5W1.5Nb14O44 Anode Material for High-Performance Lithium-Ion Batteries

Tao, Runming; Zhang, Tianyu; Tan, Susheng; Jafta, Charl J.; Li, Cheng; Liang, Jiyuan; Sun, Xiao-Guang; Wang, Tao; Fan, Juntian; Lu, Ziyang; Bridges, Craig A.; Suo, Xian; Do-Thanh, Chi-Linh; Dai, Sheng

doi:10.1002/aenm.202200519

Insight into the Fast-Rechargeability of a Novel Mo_1.5W_1.5Nb₁₄O₄₄ Anode Material for High-Performance Lithium-Ion Batteries

Journal Article · Fri Jul 22 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202200519· OSTI ID:1890324

Tao, Runming ^[1]; Zhang, Tianyu ^[1]; Tan, Susheng ^[2]; ^[3]; ^[3]; Liang, Jiyuan ^[4]; ^[3]; ^[3]; Fan, Juntian ^[1]; Lu, Ziyang ^[5]; ^[3]; Suo, Xian ^[6]; Do-Thanh, Chi-Linh ^[6]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Pittsburgh, PA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States); Jianghan Univ., Wuhan (China)
Univ. of Tennessee, Knoxville, TN (United States); Jiangsu Univ. (China)
Univ. of Tennessee, Knoxville, TN (United States)

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 Mo_1.5W_1.5Nb₁₄O₄₄ (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. In this work, 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 LiNi_0.5Mn_1.5O₄-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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1890324

Alternate ID(s):: OSTI ID: 1889318

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 36 Vol. 12; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
Mo1.5W1.5Nb14O44
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ionothermal synthesis
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