Tailoring the adsorption behavior of superoxide intermediates on nickel carbide enables high-rate Li–O2 batteries
Yun Liu,
Jinyan Cai,
Jianbin Zhou,
Yipeng Zang,
Xusheng Zheng,
Zixuan Zhu,
Bo Liu,
Gongming Wang,
Yitai Qian
Affiliations
Yun Liu
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China
Jinyan Cai
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China
Jianbin Zhou
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China
Yipeng Zang
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China
Xusheng Zheng
National Synchrotron Radiation Laboratory, University of Science & Technology of China, Hefei, 230029, PR China
Zixuan Zhu
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China
Bo Liu
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China; Corresponding authors.
Gongming Wang
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China; Corresponding authors.
Yitai Qian
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemistry, University of Science & Technology of China, Hefei, Anhui, 230026, PR China; Corresponding authors.
Probing the relationship between the adsorption of superoxide species and the kinetics of Li–O2 chemistry is critical for designing superior oxygen electrodes for the Li–O2 battery, yet the modulation essence, especially at the atomic level, remains little understood. Herein, we reveal that the adsorption behaviors of superoxide species can be effectively regulated via a core-induced interfacial charge interaction, and we find that moderate adsorption strength can enable superior rate capability in a Li–O2 battery. More importantly, operando X-ray absorption near-edge structure and surface-enhanced Raman spectroscopy provide tools to monitor in situ the evolution of the superoxide intermediates and the electronic states of the catalyst's metal sites during the discharge and charge processes, and correlate these with the surface adsorption states. The concept of tuning adsorption behavior through interfacial charge engineering could open up new opportunities to further advance the development of the Li–O2 battery and beyond.
