Nitrogen-Centered Organic Salts Enable Stable Lithium-Ion Supply for High-Energy-Density Batteries.

Journal: Journal of the American Chemical Society
Published Date: Aug 27, 2025

Abstract

Compensating lithium (Li) ions for high-energy-density batteries is essential, as the anodes such as silicon-based materials present up to 20% Li-ion loss in the initial cycle. Current Li-ion supply molecules present side reactions with battery components and lead to undesirable gas generation due to the intrinsic electrochemical mechanism. To address this, we report the design of a nitrogen (N)-centered organic salt, lithium-benzimidazol-2-one (LiNCHO), capable of supplying Li-ions without damaging the battery chemical environment and effectively protecting the Ni-rich cathode surface. This molecule, discovered through semisupervised machine learning, undergoes a two-step anodic reaction through a free radical pathway, releasing Li-ions and forming an electrolyte additive, benzimidazolone (CHNO), to suppressing transition metal dissolution of the LiNiCoMnO (NCM811) cathode. No gases were generated in this process. The complete conversion of LiNCHO and effective protection of NCM811 were confirmed by spectroscopic and microscopic characterizations. The utilization of LiNCHO effectively increased the capacity of a silicon monoxide (SiO)/C|NCM811 pouch cell from 186.7 to 205.5 mAh g, and the cell delivered an 84.1% capacity retention after 500 cycles, opening up an avenue to design a N-centered oxidation reaction mechanism for Li-ion supply in high-energy-density batteries.

Authors

  • Ziyang Kang
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Institute of Fiber Materials and Devices, Research Center of AI for Polymer Science, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200433, China.
  • Shengfei Wang
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Institute of Fiber Materials and Devices, Research Center of AI for Polymer Science, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200433, China.
  • Guanbin Wu
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Institute of Fiber Materials and Devices, Collaborative Innovation Center of Chemistry for Energy Materials, Research Center of AI for Polymer Science, Fudan University, Shanghai, 200438, China.
  • Shu Chen
    Department of Materials, London Centre for Nanotechnology, Imperial College London SW3 UK.
  • Zilong Zheng
    Big Data Center, The Seventh Affiliated Hospital of Sun Yat-sen University, Shenzhen 518107, P.R. China.
  • Wenwen Wang
    Department of Computer Science, University of Georgia, Athens, GA, USA.
  • Xinwei Du
    Pediatric Thoracic and Cardiovascular Surgery, Shanghai Children's Medical Center, School of Medicine and National Children's Medical Center, Shanghai Jiao Tong University.
  • Huajing Li
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Institute of Fiber Materials and Devices, Research Center of AI for Polymer Science, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200433, China.
  • Mengyao Zhu
    Department of Orthodontics, School of Stomatology, Capital Medical University, Beijing 100050, China.
  • Huisheng Peng
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Institute of Fiber Materials and Devices, Research Center of AI for Polymer Science, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200433, China.
  • Yue Gao
    Institute of Medical Technology, Peking University Health Science Center, Beijing, China.

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