Zhu Zhuo, Lv Qingliang, Ni Youxuan, Gao Suning, Geng Jiarun, Liang Jing, Li Fujun
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Center (RECAST), College of Chemistry, Nankai University, Tianjin, 300071, China.
Haihe Laboratory of Sustainable Chemical Transformations.
Angew Chem Int Ed Engl. 2022 Mar 14;61(12):e202116699. doi: 10.1002/anie.202116699. Epub 2022 Jan 28.
Li-O batteries have aroused considerable interest in recent years, however they are hindered by high kinetic barriers and large overvoltages at cathodes. Herein, a step-scheme (S-scheme) junction with hematite on carbon nitride (Fe O /C N ) is designed as a bifunctional catalyst to facilitate oxygen redox for a visible-light-involved Li-O battery. The internal electric field and interfacial Fe-N bonding in the heterojunction boost the separation and directional migration of photo-carriers to establish spatially isolated redox centers, at which the photoelectrons on C N and holes on Fe O remarkably accelerate the discharge and charge kinetics. These enable the Li-O battery with Fe O /C N to present an elevated discharge voltage of 3.13 V under illumination, higher than the equilibrium potential 2.96 V in the dark, and a charge voltage of 3.19 V, as well as superior rate capability and cycling stability. This work will shed light on rational cathode design for metal-O batteries.
近年来,锂氧电池引起了人们的广泛关注,然而它们受到阴极处高动力学势垒和大过电压的阻碍。在此,设计了一种在氮化碳上负载赤铁矿的阶梯型(S型)异质结(Fe₂O₃/C₃N₄)作为双功能催化剂,以促进可见光参与的锂氧电池中的氧氧化还原反应。异质结中的内建电场和界面Fe-N键促进了光生载流子的分离和定向迁移,从而建立了空间隔离的氧化还原中心,在该中心处,C₃N₄上的光电子和Fe₂O₃上的空穴显著加速了充放电动力学。这些使得具有Fe₂O₃/C₃N₄的锂氧电池在光照下呈现出3.13 V的升高放电电压,高于黑暗中的平衡电位2.96 V,充电电压为3.19 V,以及优异的倍率性能和循环稳定性。这项工作将为金属氧电池的合理阴极设计提供启示。