Single-Atom Ru Implanted on Co3 O4 Nanosheets as Efficient Dual-Catalyst for Li-CO2 Batteries

• Published in: Advanced science 2021-12, Vol.8 (23), p.e2102550
• Main Authors: Lian, Zheng, Lu, Youcai, Wang, Chunzhi, Zhu, Xiaodan, Ma, Shiyu, Li, Zhongjun, Liu, Qingchao, Zang, Shuangquan
• Format: Article
• Language: English
• ISSN: 2198-3844; 2198-3844
• DOI: 10.1002/advs.202102550

Li-CO2 battery has attracted extensive attention and research due to its super high theoretical energy density and its ability to fix greenhouse gas CO2 . However, the slow reaction kinetics during discharge/charge seriously limits its development. Hence, a simple cation exchange strategy is developed to introduce Ru atoms onto a Co3 O4 nanosheet array grown on carbon cloth (SA Ru-Co3 O4 /CC) to prepare a single atom site catalyst (SASC) and successfully used in Li-CO2 battery. Li-CO2 batteries based on SA Ru-Co3 O4 /CC cathode exhibit enhanced electrochemical performances including low overpotential, ultra high capacity, and long cycle life. Density functional theory calculations reveal that single atom Ru as the driving force center can significantly enhance the intrinsic affinity for key intermediates, thus enhancing the reaction kinetics of CO2 reduction reaction in Li-CO2 batteries, and ultimately optimizing the growth pathway of discharge products. In addition, the Bader charge analysis indicates that Ru atoms as electron-deficient centers can enhance the catalytic activity of SA Ru-Co3 O4 /CC cathode for the CO2 evolution reaction. It is believed that this work has important implications for the development of new SASCs and the design of efficient catalyst for Li-CO2 batteries.Li-CO2 battery has attracted extensive attention and research due to its super high theoretical energy density and its ability to fix greenhouse gas CO2 . However, the slow reaction kinetics during discharge/charge seriously limits its development. Hence, a simple cation exchange strategy is developed to introduce Ru atoms onto a Co3 O4 nanosheet array grown on carbon cloth (SA Ru-Co3 O4 /CC) to prepare a single atom site catalyst (SASC) and successfully used in Li-CO2 battery. Li-CO2 batteries based on SA Ru-Co3 O4 /CC cathode exhibit enhanced electrochemical performances including low overpotential, ultra high capacity, and long cycle life. Density functional theory calculations reveal that single atom Ru as the driving force center can significantly enhance the intrinsic affinity for key intermediates, thus enhancing the reaction kinetics of CO2 reduction reaction in Li-CO2 batteries, and ultimately optimizing the growth pathway of discharge products. In addition, the Bader charge analysis indicates that Ru atoms as electron-deficient centers can enhance the catalytic activity of SA Ru-Co3 O4 /CC cathode for the CO2 evolution reaction. It is believed that this work has impo