<p>Low-cost and high-safety aqueous Zn-I<sub>2</sub> batteries attract extensive attention for large-scale energy storage systems. However, polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capability and severe capacity decay. Herein, a three-dimensional polyaniline is wrapped by carboxyl-carbon nanotubes (denoted as C-PANI) which is designed as a catalytic cathode to effectively boost iodine conversion with suppressed polyiodide shuttling, thereby improving Zn-I<sub>2</sub> batteries. Specifically, carboxyl-carbon nanotubes serve as a proton reservoir for more protonated –NH<sup>+</sup> = sites in PANI chains, achieving a direct I<sup>0</sup>/I<sup>−</sup> reaction for suppressed polyiodide generation and Zn corrosion. Attributing to this “proton-iodine” regulation, catalytic protonated C-PANI strongly fixes electrolytic iodine species and stores proton ions simultaneously through reversible –N = /–NH<sup>+</sup>– reaction. Therefore, the electrolytic Zn-I<sub>2</sub> battery with C-PANI cathode exhibits an impressive capacity of 420&#xa0;mAh&#xa0;g<sup>−1</sup> and ultra-long lifespan over 40,000 cycles. Additionally, a 60&#xa0;mAh pouch cell was assembled with excellent cycling stability after 100 cycles, providing new insights into exploring effective organocatalysts for superb Zn-halogen batteries.</p>

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“Proton-Iodine” Regulation of Protonated Polyaniline Catalyst for High-Performance Electrolytic Zn-I2 Batteries

  • Mengyao Liu,
  • Kovan Khasraw Abdalla,
  • Meng Xu,
  • Xueqian Li,
  • Runze Wang,
  • Qi Li,
  • Xiaoru Zhang,
  • Yanan Lv,
  • Yueyang Wang,
  • Xiaoming Sun,
  • Yi Zhao

摘要

Low-cost and high-safety aqueous Zn-I2 batteries attract extensive attention for large-scale energy storage systems. However, polyiodide shuttling and sluggish iodine conversion reactions lead to inferior rate capability and severe capacity decay. Herein, a three-dimensional polyaniline is wrapped by carboxyl-carbon nanotubes (denoted as C-PANI) which is designed as a catalytic cathode to effectively boost iodine conversion with suppressed polyiodide shuttling, thereby improving Zn-I2 batteries. Specifically, carboxyl-carbon nanotubes serve as a proton reservoir for more protonated –NH+ = sites in PANI chains, achieving a direct I0/I reaction for suppressed polyiodide generation and Zn corrosion. Attributing to this “proton-iodine” regulation, catalytic protonated C-PANI strongly fixes electrolytic iodine species and stores proton ions simultaneously through reversible –N = /–NH+– reaction. Therefore, the electrolytic Zn-I2 battery with C-PANI cathode exhibits an impressive capacity of 420 mAh g−1 and ultra-long lifespan over 40,000 cycles. Additionally, a 60 mAh pouch cell was assembled with excellent cycling stability after 100 cycles, providing new insights into exploring effective organocatalysts for superb Zn-halogen batteries.