Wang Di, Li Linyue, Li Xiang, Han Wenjie, Dan Binbin, Li Shixuan, Liu Xiang, Wang Zhoulu, He Ping
School of energy science and engineering, Nanjing Tech University, 30 South Puzhu Road, Nanjing, 211816, PR China.
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, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, P. R. China.
ChemSusChem. 2025 Feb 16;18(4):e202401558. doi: 10.1002/cssc.202401558. Epub 2025 Jan 24.
Li-CO batteries have been recognized as an emerging technology for energy storage systems owing to their high theoretical specific energy and environmentally friendly CO fixation ability. However, their development for applications requires a high energy efficiency and long cycle-life, this is currently limited to the formation of wide-bandgap insulator LiCO during discharge. Here, nanoparticle Pd supported on reduced graphene oxide (rGO) is utilized as cathodes for Li-CO batteries, Pd nanoparticles as active centers significantly enhance CORR/COER reaction activity, which can support the fast formation and decomposition of LiCO in organic electrolytes and achieve a high discharge capacity of 7500 mAh g. It also performs remarkably high cycling stability of over 500 cycles with a long cycle-life of 5000 hours. The observed super electrochemical performance is attributable to the thick electrode design and uniform distribution of ultrafine catalyst nanoparticle Pd. When LiCO is adsorbed on Pd particle, the Li-O bond in LiCO will be elongated due to the interactions of two nucleophilic O atoms with Pd, resulting in a weakening of the Li-O bond and activation of LiCO. Our work suggests a way to design catalysts with high activity that can be used to activate the performance of Li-CO batteries.
锂-二氧化碳电池因其高理论比能量和环境友好的二氧化碳固定能力，已被公认为是一种用于储能系统的新兴技术。然而，其应用开发需要高能量效率和长循环寿命，目前这受到放电过程中宽带隙绝缘体碳酸锂形成的限制。在此，负载在还原氧化石墨烯（rGO）上的纳米颗粒钯被用作锂-二氧化碳电池的阴极，钯纳米颗粒作为活性中心显著提高了二氧化碳还原反应/二氧化碳析出反应活性，这能够支持有机电解质中碳酸锂的快速形成和分解，并实现7500 mAh g的高放电容量。它还具有超过500次循环的显著高循环稳定性，循环寿命长达5000小时。观察到的超电化学性能归因于厚电极设计和超细催化剂纳米颗粒钯的均匀分布。当碳酸锂吸附在钯颗粒上时，由于两个亲核氧原子与钯的相互作用，碳酸锂中的锂-氧键将被拉长，导致锂-氧键减弱和碳酸锂活化。我们的工作提出了一种设计高活性催化剂的方法，可用于激活锂-二氧化碳电池的性能。
