Li Wei, Zhang Menghang, Sun Xinyi, Sheng Chuanchao, Mu Xiaowei, Wang Lei, He Ping, Zhou Haoshen
Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, PR China.
Nat Commun. 2024 Jan 27;15(1):803. doi: 10.1038/s41467-024-45087-4.
Li-CO batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO often results in the formation of LiCO, causing a dip in output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to the cathode via a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents the shuttle effect and sluggish kinetics associated with soluble redox mediators. Results show that the electrochemically reduced Cu(I) solid redox mediator efficiently captures CO, facilitating LiCO formation through a dimerization reaction involving a dimeric oxalate intermediate. The Li-CO battery employing the Cu(II) solid redox mediator boasts a higher discharge voltage of 2.8 V, a lower charge potential of 3.7 V, and superior cycling performance over 400 cycles. Simultaneously, the successful development of a Li-CO pouch battery propels metal-CO batteries closer to practical application.
锂-CO电池为将温室气体转化为电能提供了一条有前景的途径。然而，直接电催化还原惰性CO的固有挑战常常导致LiCO的形成，从而使输出电压和能量效率下降。我们的创新方法涉及通过苯-1,3,5-三羧酸的Cu(II)配位化合物固定在阴极上的固体氧化还原介质。该技术有效地规避了与可溶性氧化还原介质相关的穿梭效应和缓慢动力学。结果表明，电化学还原的Cu(I)固体氧化还原介质能有效捕获CO，通过涉及二聚草酸中间体的二聚反应促进LiCO的形成。采用Cu(II)固体氧化还原介质的锂-CO电池具有2.8 V的较高放电电压、3.7 V的较低充电电位以及超过400次循环的卓越循环性能。同时，锂-CO软包电池的成功开发使金属-CO电池更接近实际应用。
