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<p>Rechargeable aluminum batteries (RABs) represent a promising candidate for large-scale energy storage due to their high theoretical capacity, inherent safety, and abundant reserves of Al. However, their practical deployment remains constrained by conventional AlCl<sub>3</sub>-based ionic liquid electrolytes, which exhibit high production cost, uncontrolled dendrite growth, and severe anode corrosion. Here, a molecular-level ligand engineering strategy is proposed, employing nitrogen-containing cyclic amides with tunable N–H functionalities to modulate the coordination environment of deep eutectic electrolyte (DEE). Combined experimental and theoretical investigations reveal that the α-pyrrolidone-based DEE (PDEE) possesses a wider electrochemical window, higher ionic conductivity, and lower polarization. Moreover, the precise N–H regulation optimizes cationic ligand and the chloraluminate anion interactions and accelerates ion transport to facilitate uniform Al deposition without dendrites. The amine functionalities facilitate the <i>in situ</i> construction of a uniform inorganic-organic bilayer solid electrolyte interphase, effectively mitigating anode corrosion and enhancing long-term interfacial stability. As a result, the Al//Al symmetric battery with the PDEE achieves stable cycling for over 2000 h, while the Al-graphite full battery demonstrates little capacity decay after 6000 cycles. This study establishes that ligand molecular engineering offers an effective strategy for optimizing DEE, enabling the development of durable and high-performance RABs.</p>

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Molecular tailoring modulates coordination of deep eutectic electrolytes for dendrite-free rechargeable aluminum batteries

  • 期刊论文

  • 发表日期：

    2026年5月6日

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  • Tianshuo Zhao,
  • Fei Wang,
  • Zhaohui Yang,
  • Zhao Li,
  • Kaiqi Li,
  • Biao Ran,
  • Yonghong Qin,
  • Yizhou Dong,
  • Ting Wang,
  • Jiao Zhang,
  • Chaopeng Fu

摘要

Rechargeable aluminum batteries (RABs) represent a promising candidate for large-scale energy storage due to their high theoretical capacity, inherent safety, and abundant reserves of Al. However, their practical deployment remains constrained by conventional AlCl3-based ionic liquid electrolytes, which exhibit high production cost, uncontrolled dendrite growth, and severe anode corrosion. Here, a molecular-level ligand engineering strategy is proposed, employing nitrogen-containing cyclic amides with tunable N–H functionalities to modulate the coordination environment of deep eutectic electrolyte (DEE). Combined experimental and theoretical investigations reveal that the α-pyrrolidone-based DEE (PDEE) possesses a wider electrochemical window, higher ionic conductivity, and lower polarization. Moreover, the precise N–H regulation optimizes cationic ligand and the chloraluminate anion interactions and accelerates ion transport to facilitate uniform Al deposition without dendrites. The amine functionalities facilitate the in situ construction of a uniform inorganic-organic bilayer solid electrolyte interphase, effectively mitigating anode corrosion and enhancing long-term interfacial stability. As a result, the Al//Al symmetric battery with the PDEE achieves stable cycling for over 2000 h, while the Al-graphite full battery demonstrates little capacity decay after 6000 cycles. This study establishes that ligand molecular engineering offers an effective strategy for optimizing DEE, enabling the development of durable and high-performance RABs.