A 2.75 V ammonium‐based dual‐ion battery

• Published in: Angewandte Chemie International Edition Vol. 61; no. 51; pp. e202212941 - n/a
• Main Authors: Zhao, Zhiming, Lei, Yongjiu, Shi, Lin, Tian, Zhengnan, Hedhili, Mohamed N., Khan, Yusuf, Alshareef, Husam N.
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 19.12.2022
• Edition: International ed. in English
• Subjects: Ammonium; Batteries; Cathodes; Diimide; Dual-Ion Battery; Electric potential; Graphite; Heavy metals; High-Voltage Electrolyte; Intercalation; Metal-Free Battery; Organic Ammonium-Ion Battery; Voltage; Metal-Free Battery; Organic Ammonium-Ion Battery; Dual-Ion Battery; High-Voltage Electrolyte
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202212941

The popular metal‐ion batteries (MIBs) suffer from environmental and economic issues because of their heavy dependency on nonrenewable metals. Here, we propose a metal‐free ammonium (NH4+)‐based dual‐ion battery with a record‐breaking operation voltage of 2.75 V. The working mechanism of this sustainable battery involves the reversible anion (PF6−) intercalation chemistry in graphite cathode and NH4+ intercalation behavior in PTCDI (3,4,9,10‐perylenetetracarboxylic diimide) anode. This new battery configuration successfully circumvented the reduction susceptibility of NH4+ and the lack of mature NH4+‐rich cathodes for NH4+ ion batteries (AIBs). The customized organic NH4+ electrolyte endows the graphite||PTCDI full battery with durable longevity (over 1000 cycles) and a high energy density (200 Wh kg−1). We show that the development of AIBs should be high‐voltage‐oriented while circumventing low operation potential to avoid NH4+ reduction. We bypassed the reduction susceptibility of NH4+ and promoted the NH4+ ion battery toward a record‐breaking operation voltage of 2.75 V by co‐utilizing the storage of the other significant charge carrier in electrolytes, viz, anions, realizing a high‐voltage metal‐free battery.