<p>The practical implementation of aqueous zinc-ion batteries (AZIBs) faces significant challenges stemming from zinc anode instability, including corrosion, hydrogen evolution reaction (HER), parasitic byproduct formation, and uncontrolled dendrite growth. To comprehensively address these issues, we developed a multifunctional cerium-based metal-organic framework (Ce-MOF) coating for zinc anodes; the coating features an ordered porous structure and inherent properties that mitigate HER, suppress side reactions, and inhibit dendrite formation. The symmetric cells using Ce-MOF/Zn demonstrate exceptional cycling stability for over 2060 h at 0.5 mA cm<sup>−2</sup> with low hysteresis polarization of 26 mV. In full cell, with I<sub>2</sub>@AC cathode, the Ce-MOF/Zn∥I<sub>2</sub>@AC achieved outstanding cycling stability of 28550 cycles at 5 A g<sup>−1</sup>, with 91% capacity retention (109.6 mAh g<sup>−1</sup>). Through integrated characterization employing <i>in-situ</i> optical microscopy, <i>ex-situ</i> XRD, SEM, and DFT calculations, we elucidate the multifunctional mechanism: the Ce-MOF coating facilitates preferential (002)-oriented Zn deposition to suppress dendrites, reduces Zn<sup>2+</sup> desolvation energy to enhance deposition kinetics, and modulates interfacial chemistry to mitigate HER and corrosion. This work establishes Ce-MOF coatings as a simple yet powerful strategy for developing high performance zinc anodes, providing critical insights for advancing practical AZIB technologies.</p>

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A multifunctional cerium-based metal-organic framework coating for a dendrite-free and highly stable zinc metal anode

  • Chang Shu,
  • Yilong Xu,
  • Yongfeng Huang,
  • Yunlin An,
  • Yunqing Liu,
  • Chen Zhang,
  • Xiaoyu Zhang,
  • Jianchao Sun,
  • Feiyu Kang,
  • Xueqin Sun,
  • Fuyi Jiang,
  • Wenbao Liu

摘要

The practical implementation of aqueous zinc-ion batteries (AZIBs) faces significant challenges stemming from zinc anode instability, including corrosion, hydrogen evolution reaction (HER), parasitic byproduct formation, and uncontrolled dendrite growth. To comprehensively address these issues, we developed a multifunctional cerium-based metal-organic framework (Ce-MOF) coating for zinc anodes; the coating features an ordered porous structure and inherent properties that mitigate HER, suppress side reactions, and inhibit dendrite formation. The symmetric cells using Ce-MOF/Zn demonstrate exceptional cycling stability for over 2060 h at 0.5 mA cm−2 with low hysteresis polarization of 26 mV. In full cell, with I2@AC cathode, the Ce-MOF/Zn∥I2@AC achieved outstanding cycling stability of 28550 cycles at 5 A g−1, with 91% capacity retention (109.6 mAh g−1). Through integrated characterization employing in-situ optical microscopy, ex-situ XRD, SEM, and DFT calculations, we elucidate the multifunctional mechanism: the Ce-MOF coating facilitates preferential (002)-oriented Zn deposition to suppress dendrites, reduces Zn2+ desolvation energy to enhance deposition kinetics, and modulates interfacial chemistry to mitigate HER and corrosion. This work establishes Ce-MOF coatings as a simple yet powerful strategy for developing high performance zinc anodes, providing critical insights for advancing practical AZIB technologies.