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<p>Lithium-carbon dioxide batteries hold great promise for high-energy-density storage applications. However, advancing this technology as a sustainable alternative to Li-ion systems requires a deeper understanding of the underlying reaction mechanisms, which remain elusive. A key challenge stems from the added complexity introduced by the presence of oxygen in CO<sub>2</sub> environment. In this study, we employ a stable Cu<sub>3</sub>(VBi)<sub>0.5</sub>Se<sub>4</sub> mid-entropy catalyst and conduct comprehensive investigation to uncover the underlying reaction mechanisms in Li-CO<sub>2</sub> batteries under varying CO<sub>2</sub>/O<sub>2</sub> ratios. Under pure CO<sub>2</sub> conditions, the battery shows extended rechargeability, sustaining up to 1200 cycles at a current density of 0.2 mA/cm<sup>2</sup> and capacity of 0.1 mAh/cm<sup>2</sup>. However, at high current densities, the discharge potential drops significantly (below 2.0 V), primarily due to sluggish reaction kinetics caused by solid carbon formation. Interestingly, introducing O<sub>2</sub> mitigates this limitation, leading to a 58% increase of the discharge potential (from 1.7 V to 2.7 V) at the current density of 0.8 mA/cm<sup>2</sup>, signifying a substantial boost in energy output. Our results reveal that the reactions follow distinct pathways, shifting from surface- to solution-based mechanism, and even exhibit coexistence of both mechanisms, depending on the CO<sub>2</sub>/O<sub>2</sub> ratio. These findings offer useful insights for designing sustainable Li-gas batteries utilizing CO<sub>2</sub> and O<sub>2</sub> mixtures.</p>

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Pathways for sustainable reaction kinetics in Li-CO2 batteries

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月17日

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  • Ilias Papailias,
  • Arash Namaeighasemi,
  • Musawenkosi K. Ncube,
  • Roshan Y. Nemade,
  • Naveen Dandu,
  • Nikhil Rai,
  • Syed Ibrahim Gnani Peer Mohamed,
  • Hessam Shahbazi,
  • Suchit Sarin,
  • Ahmad Jaradat,
  • Shahriar Namvar,
  • Pardis Seraji,
  • Vikas Berry,
  • Arunkumar Subramanian,
  • Jeffrey Shield,
  • Siamak Nejati,
  • Anh T. Ngo,
  • Larry A. Curtiss,
  • Amin Salehi-Khojin

摘要

Lithium-carbon dioxide batteries hold great promise for high-energy-density storage applications. However, advancing this technology as a sustainable alternative to Li-ion systems requires a deeper understanding of the underlying reaction mechanisms, which remain elusive. A key challenge stems from the added complexity introduced by the presence of oxygen in CO2 environment. In this study, we employ a stable Cu3(VBi)0.5Se4 mid-entropy catalyst and conduct comprehensive investigation to uncover the underlying reaction mechanisms in Li-CO2 batteries under varying CO2/O2 ratios. Under pure CO2 conditions, the battery shows extended rechargeability, sustaining up to 1200 cycles at a current density of 0.2 mA/cm2 and capacity of 0.1 mAh/cm2. However, at high current densities, the discharge potential drops significantly (below 2.0 V), primarily due to sluggish reaction kinetics caused by solid carbon formation. Interestingly, introducing O2 mitigates this limitation, leading to a 58% increase of the discharge potential (from 1.7 V to 2.7 V) at the current density of 0.8 mA/cm2, signifying a substantial boost in energy output. Our results reveal that the reactions follow distinct pathways, shifting from surface- to solution-based mechanism, and even exhibit coexistence of both mechanisms, depending on the CO2/O2 ratio. These findings offer useful insights for designing sustainable Li-gas batteries utilizing CO2 and O2 mixtures.