Electrochemistry Enabled Heterostructure with High Tap Density for Ultrahigh Power Na-Ion Capacitors

Developing electrode materials with high tap density, low cost, and superior performance poses a formidable challenge in electrochemistry. The impressive performance exhibited by most electrodes comes at the expense of tap density and cost, severely limiting their practical applications. Here, combining computational and experimental results, an approach for the electrode materials with high tap density and rich heterostructure (Cu2S/Na2Sn) from cheap copper smelting slag enabled by an electrochemical process is proposed, reducing the diffusion energy barrier from 0.82 to 0.28 eV for Na+, as well as delivering an impressively high tap density of 3.32 g cm-3. Furthermore, the electrochemical activation process that irreversibly generates more stable Cu2S and Na2Sn after the first charge progress of parent materials is also revealed by in/ex situ analytical techniques. As expected, assembled sodium ion capacitors (SICs) achieve high energy density (74.4 Wh kg-1) at high power density (20 000 W kg-1) with outstanding capacity retention of 81.5% after 10 000 cycles, delivering over 76% of its energy density in 13.4 s, which surpasses the performance achieved by state-of-the-art SICs. This work not only provides novel insights into irreversibly conversion-type anodes but also introduces a method for efficient value-added utilization of smelting slag. The study demonstrates a novel electrochemical behavior of CuS anodes and reveals the enhanced Na+ storage capability by electrochemistry enabled Cu2S/Na2Sn heterostructure and sulfur vacancies. Consequently, the assembled sodium ion capacior (SIC) achieves an impressive energy density of 74.4 Wh kg-1 at remarkable power density of 20 000 W kg-1 with an ultralong cycling life exceeding 10 000 cycles.image