A High‐Voltage <i>n‐</i>type Organic Cathode Materials Enabled by Tetraalkylammonium Complexing Agents for Aqueous Zinc‐Ion Batteries

Authors: Jaehyun Park, Abigail M. Houser, Shiyu Zhang

Published: 2024-10-25

DOI: 10.1002/adma.202409946

Source: Full article


Abstract

AbstractTetrabutylammonium (TBA) salt of hexacyano‐substituted cyclopropane dianion (Cp(CN)62−) is prepared through a facile two‐step synthetic protocol from commercially available materials and fully characterized as a high‐voltage n‐type organic cathode in rechargeable aqueous zinc‐ion batteries (AZIBs). The addition of tetrabutylammonium triflate (TBAOTf) to the electrolyte mitigates dissolution issues, leading to enhanced cycling stability. Remarkably, the Cp(CN)62− cathode demonstrates a high discharge voltage of 1.43 V in AZIBs and retains 85% of its capacity after 1000 cycles at a high loading of 10 mg cm−2 and a cycling rate of 10C. These results, combined with spectroscopic analyses, elucidate a reversible two‐electron redox process of Cp(CN)62− facilitated by the insertion/de‐insertion of TBA cation. These findings underscore the potential of Cp(CN)62− as a conversion‐based n‐type cathode in energy storage applications.