<p>Lithium metal is considered the ideal anode material for achieving high-energy-density lithium-ion batteries due to its extremely high theoretical specific capacity and low redox potential. However, the uncontrollable growth of lithium dendrites and the drastic volume expansion during cycling pose significant safety risks and severely limit the practical application of lithium metal batteries. To address the aforementioned issues, this study developed a multi-walled carbon nanotube/Al<sub>2</sub>O<sub>3</sub> (MWCNTs/Al<sub>2</sub>O<sub>3</sub>) composite material via a hydrothermal-calcination method and constructed it into a three-dimensional conductive framework for lithium metal anodes. The composite framework combines the high electronic conductivity of MWCNTs with the excellent interfacial stability of Al<sub>2</sub>O<sub>3</sub>, serving as an effective host for lithium metal. It significantly reduces local current density, promotes uniform lithium nucleation and deposition, thereby effectively mitigating volume expansion and suppressing lithium dendrite growth. The results show that under a current density of 1&#xa0;mA cm<sup>− 2</sup> and an areal capacity of 1 mAh cm<sup>− 2</sup>, the LiMWCNTs/Al<sub>2</sub>O<sub>3</sub> symmetric cell exhibits a stable cycling lifetime exceeding 1300&#xa0;h, which is significantly longer than the 410&#xa0;h observed for the pure Li symmetric cell. Moreover, full cells based on this anode, LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>||LiMWCNTs/Al<sub>2</sub>O<sub>3</sub> full cells, exhibit excellent rate performance and significantly enhanced cycling stability. At a current density of 1&#xa0;C, they deliver a reversible capacity of 139.2 mAh g<sup>− 1</sup> and retain 84.3% of the capacity after 400 cycles, which is markedly higher than the 62.3% retention observed for LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>||Li full cells. This work proposes a simple yet effective three-dimensional framework design strategy, providing a new approach for constructing dendrite-free, long-life, and high-performance lithium metal anodes, and offering a feasible and innovative solution for the development of high-energy-density lithium metal batteries.</p>

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3D MWCNTs framework anchored with Li-Philic nano-Al2O3 for controlled Lithium deposition and extended cycling of Lithium metal anodes

  • Liming Wang,
  • Jun Peng,
  • Jun Yang,
  • Anmin Huang,
  • Haiyang Yang,
  • Yuhan Liu,
  • Ziyang Su,
  • Shiling Zhang,
  • Qing Peng

摘要

Lithium metal is considered the ideal anode material for achieving high-energy-density lithium-ion batteries due to its extremely high theoretical specific capacity and low redox potential. However, the uncontrollable growth of lithium dendrites and the drastic volume expansion during cycling pose significant safety risks and severely limit the practical application of lithium metal batteries. To address the aforementioned issues, this study developed a multi-walled carbon nanotube/Al2O3 (MWCNTs/Al2O3) composite material via a hydrothermal-calcination method and constructed it into a three-dimensional conductive framework for lithium metal anodes. The composite framework combines the high electronic conductivity of MWCNTs with the excellent interfacial stability of Al2O3, serving as an effective host for lithium metal. It significantly reduces local current density, promotes uniform lithium nucleation and deposition, thereby effectively mitigating volume expansion and suppressing lithium dendrite growth. The results show that under a current density of 1 mA cm− 2 and an areal capacity of 1 mAh cm− 2, the LiMWCNTs/Al2O3 symmetric cell exhibits a stable cycling lifetime exceeding 1300 h, which is significantly longer than the 410 h observed for the pure Li symmetric cell. Moreover, full cells based on this anode, LiNi0.8Co0.1Mn0.1O2||LiMWCNTs/Al2O3 full cells, exhibit excellent rate performance and significantly enhanced cycling stability. At a current density of 1 C, they deliver a reversible capacity of 139.2 mAh g− 1 and retain 84.3% of the capacity after 400 cycles, which is markedly higher than the 62.3% retention observed for LiNi0.8Co0.1Mn0.1O2||Li full cells. This work proposes a simple yet effective three-dimensional framework design strategy, providing a new approach for constructing dendrite-free, long-life, and high-performance lithium metal anodes, and offering a feasible and innovative solution for the development of high-energy-density lithium metal batteries.