Engineering Dual Single‐Atom Sites on 2D Ultrathin N‐doped Carbon Nanosheets Attaining Ultra‐Low‐Temperature Zinc‐Air Battery

• Published in: Angewandte Chemie International Edition Vol. 61; no. 12; pp. e202115219 - n/a
• Main Authors: Cui, Tingting, Wang, Yun‐Peng, Ye, Tong, Wu, Jiao, Chen, Zhiqiang, Li, Jiong, Lei, Yongpeng, Wang, Dingsheng, Li, Yadong
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 14.03.2022
• Edition: International ed. in English
• Subjects: Air temperature; Bifunctional electrocatalyst; Carbon; Catalysts; Catalytic activity; Chemical reduction; Density functional theory; Dual single-atom catalyst; Low temperature; Manganese; Mass transfer; Metal air batteries; Nanosheets; Oxygen; Oxygen evolution reactions; Oxygen reduction reactions; Room temperature; Specific capacity; Zinc; Zn-air battery; Bifunctional electrocatalyst; Nanosheets; Zn-air battery; Dual single-atom catalyst; Low-temperature
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202115219

Herein, a novel dual single‐atom catalyst comprising adjacent Fe‐N4 and Mn‐N4 sites on 2D ultrathin N‐doped carbon nanosheets with porous structure (FeMn‐DSAC) was constructed as the cathode for a flexible low‐temperature Zn‐air battery (ZAB). FeMn‐DSAC exhibits remarkable bifunctional activities for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Control experiments and density functional theory calculations reveal that the catalytic activity arises from the cooperative effect of the Fe/Mn dual‐sites aiding *OOH dissociation as well as the porous 2D nanosheet structure promoting active sits exposure and mass transfer during the reaction process. The excellent bifunctional activity of FeMn‐DSAC enables the ZAB to operate efficiently at ultra‐low temperature of −40 °C, delivering 30 mW cm−2 peak power density and retaining up to 86 % specific capacity from the room temperature counterpart. A Fe/Mn dual single‐atom catalyst with an excellent bifunctional activity is prepared as the cathode for a flexible low‐temperature Zn‐air battery (ZAB). Profiting from the combined Fe/Mn dual‐site effect as well as the porous 2D nanosheet structure, the ZAB could operate efficiently at the ultra‐low temperature of −40 °C.