Chelated Metal-Organic Frameworks for Improved the Performance of High-Nickel Cathodes in Lithium-Ion Batteries

Abstract

Lithium-ion batteries have gained widespread use in various applications, including portable devices, electric vehicles, and energy storage systems. High Ni cathode, LiNixCoyMnzO2 (NCM, x >= 0.8, x+y+z=1), have garnered significant attention owing to their high energy density. However, the limited Li-ion transfer rate and transition metal cross-talk to anode pose obstacles to further improvement of electrochemical performance. To tackle these challenges, metal-organic frameworks (MOFs) with chelating agents are employed as additive materials for electrode. MOFs with chelating agents offer three key attributes: (1) Effective mitigation of transition metal cross-talk to the anode, (2) Partial desolvation of Li+ ions through MOF pores, and (3) Immobilization of anions via metal sites in the MOF. Leveraging these advantages, the chelating MOF-modified NCM cathode demonstrates reduced charge transfer resistance, both in their pristine and cycled states. In addition, they exhibit significantly improved the Li-ion diffusion coefficients after 100 cycles. These findings underscore the potential of MOFs with chelating agents as promising additive materials for enhancing the performance of LIBs. Metal-organic frameworks (MOFs) with chelating agents address challenges in lithium-ion battery performance by mitigating transition metal cross-talk, desolvating Li+ ions, and immobilizing anions. Chelating MOF-modified cathodes show reduced charge transfer resistance and enhanced lithium-ion diffusion coefficients, highlighting their promise as passivation materials for improved lithium-ion battery performance. image