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<p>The metal triazole (MTA)-based MOFs were found to preferentially adsorb O-rich species, which had enhanced electrocatalytic oxygen reduction reactions (ORR) and stabilized the O-containing species during the discharge and charge processes in Li-O<sub>2</sub> battery. However, the MOFs exhibited low electron conductivity and poor electron transfer interface in the electrocatalysis, limiting the electrocatalytic activity. To address this issue, a nanocomposite with the Co-MTA-coated carbon nanotubes (Co-MTA-C) was constructed, which formed the three-dimensional conductivity network connected with the intersecting carbon nanotube (CNT). In this composite, the electron-rich Co-MTA interacted with the highly conductive CNT, resulting in a charge redistribution. Optimized the electronic structure of the Co center through compositional modifications presented a high valence compared to the pure MOFs. In situ X-ray absorption spectroscopy revealed a direct reaction of Co sites with intermediates such as LiO<sub><i>x</i></sub>, leading to the formation of nanosheet array discharge products. The battery based on optimized Co-MTA-C demonstrated fast kinetics and superior stability, with a low overpotential of 1.13&#xa0;V, high specific capacity of 9057&#xa0;mAh&#xa0;g<sup>−1</sup>, and long-term durability of 600 cycles. It provides a facile and effective strategy for enhancing the electrocatalytic performance through rational tuning of high-conductivity substances.</p> Graphical abstract <p></p>

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Rationally tuning the oxidation state of the open active sites in Co-based MOFs to enhance the kinetics of Li-O2 batteries

  • 期刊论文

  • 发表日期：

    2025年3月17日

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  • Pei-Yuan Su,
  • Xing-Zi Zheng,
  • Si-Ao Li,
  • Jing-Shen Xu,
  • Hao-Min Jiang,
  • Qing-Yu Kong,
  • Wei-Jie Zeng,
  • Fei Jia,
  • Ji-Hao Zhang,
  • Fan Bai,
  • Wen-Li Su,
  • Jing-Le Wang,
  • Cheng Zhang,
  • Zheng-Long Wu,
  • Wen-Kai Zhang,
  • Meng-Wei Yuan

摘要

The metal triazole (MTA)-based MOFs were found to preferentially adsorb O-rich species, which had enhanced electrocatalytic oxygen reduction reactions (ORR) and stabilized the O-containing species during the discharge and charge processes in Li-O2 battery. However, the MOFs exhibited low electron conductivity and poor electron transfer interface in the electrocatalysis, limiting the electrocatalytic activity. To address this issue, a nanocomposite with the Co-MTA-coated carbon nanotubes (Co-MTA-C) was constructed, which formed the three-dimensional conductivity network connected with the intersecting carbon nanotube (CNT). In this composite, the electron-rich Co-MTA interacted with the highly conductive CNT, resulting in a charge redistribution. Optimized the electronic structure of the Co center through compositional modifications presented a high valence compared to the pure MOFs. In situ X-ray absorption spectroscopy revealed a direct reaction of Co sites with intermediates such as LiOx, leading to the formation of nanosheet array discharge products. The battery based on optimized Co-MTA-C demonstrated fast kinetics and superior stability, with a low overpotential of 1.13 V, high specific capacity of 9057 mAh g−1, and long-term durability of 600 cycles. It provides a facile and effective strategy for enhancing the electrocatalytic performance through rational tuning of high-conductivity substances.

Graphical abstract