Zhang Zhen, Bai Wen-Long, Cai Zhi-Peng, Cheng Jin-Huan, Kuang Hua-Yi, Dong Bo-Xu, Wang Yu-Bo, Wang Kai-Xue, Chen Jie-Sheng
Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Zhiyuan College, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16404-16408. doi: 10.1002/anie.202105892. Epub 2021 Jun 15.
Li-CO batteries are regarded as next-generation high-energy-density electrochemical devices. However, the greatest challenge arises from the formation of the discharge product, Li CO , which would accumulate and deactivate heterogenous catalysts to cause huge polarization. Herein, Ru(bpy) Cl was employed as a solution-phase catalyst for Li-CO batteries and proved to be the most effective one screened so far. Spectroscopy and electrochemical analyses elucidate that the Ru center could interact with both CO and amorphous Li C O intermediate, thus promoting electroreduction process and delaying carbonate transformation. As a result, the charge potential is reduced to 3.86 V and over 60 discharge/charge cycles are achieved with a fixed capacity of 1000 mAh g at a current density of 300 mA g . Our work provides a new avenue to improve the electrochemical performance of Li-CO batteries with efficient mobile catalysts.
锂-二氧化碳电池被视为下一代高能量密度的电化学装置。然而，最大的挑战来自放电产物Li₂CO₃的形成，它会积累并使非均相催化剂失活，从而导致巨大的极化。在此，Ru(bpy)₃Cl₂被用作锂-二氧化碳电池的溶液相催化剂，并且被证明是迄今为止筛选出的最有效的催化剂。光谱和电化学分析表明，Ru中心可以与CO和无定形Li₂C₂O₄中间体相互作用，从而促进电还原过程并延缓碳酸盐转化。结果，充电电位降低到3.86 V，在300 mA g⁻¹的电流密度下，以1000 mAh g⁻¹的固定容量实现了60多次充放电循环。我们的工作为利用高效移动催化剂提高锂-二氧化碳电池的电化学性能提供了一条新途径。
