A Site‐Selective Doping Strategy of Carbon Anodes with Remarkable K‐Ion Storage Capacity

• Published in: Angewandte Chemie International Edition Vol. 59; no. 11; pp. 4448 - 4455
• Main Authors: Zhang, Wenli, Cao, Zhen, Wang, Wenxi, Alhajji, Eman, Emwas, Abdul‐Hamid, Costa, Pedro M. F. J., Cavallo, Luigi, Alshareef, Husam N.
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 09.03.2020
• Edition: International ed. in English
• Subjects: adsorption energy; anodes; carbon; Carbonaceous materials; Copolymers; Doping; Ion storage; Nitrogen; nitrogen doping; Potassium; potassium-ion batteries; Pyrolysis; Rechargeable batteries; Storage capacity; Strategy; anodes; potassium-ion batteries; carbon; nitrogen doping; adsorption energy
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.201913368

The limited potassium‐ion intercalation capacity of graphite hampers development of potassium‐ion batteries (PIB). Edge‐nitrogen doping is an effective approach to enhance K‐ion storage in carbonaceous materials. One shortcoming is the lack of precise control over producing the edge‐nitrogen configuration. Here, a molecular‐scale copolymer pyrolysis strategy is used to precisely control edge‐nitrogen doping in carbonaceous materials. This process results in defect‐rich, edge‐nitrogen doped carbons (ENDC) with a high nitrogen‐doping level (up to 10.5 at %) and a high edge‐nitrogen ratio (87.6 %). The optimized ENDC exhibits a high reversible capacity of 423 mAh g−1, a high initial Coulombic efficiency of 65 %, superior rate capability, and long cycle life (93.8 % retention after three months). This strategy can be extended to design other edge‐heteroatom‐rich carbons through pyrolysis of copolymers for efficient storage of various mobile ions. Edge contributes more: A molecular scale edge‐nitrogen doping method is developed for synthesizing highly edge‐nitrogen‐doped carbons. This doped carbon shows a high nitrogen doping ratio of 10.5 at % (87.6 % edge‐nitrogen ratio), and a high, reversible, stable K‐ion storage capacity of 423 mAh g−1.