Simultaneous Tailoring of Chemical Composition and Morphology Configuration in Metal Hexacyanoferrate for Ultrafast and Durable Sodium-Ion Storage

Angew Chem Int Ed Engl. 2024 Sep 17:e202414302. doi: 10.1002/anie.202414302. Online ahead of print.

Abstract

Metal hexacyanoferrates (MHCFs) with adjustable composition and open framework structures have been considered as intriguing cathode materials for sodium-ion batteries (SIBs). Exploiting MHCFs with ultrafast and durable sodium storage capability as well as comparable capacity is always a goal that many investigators pursue, but remains challenging. Herein, simultaneous tailoring of chemical composition and morphology configuration is carried out to design a hollow monoclinic high-entropy MHCF (HMHE-HCF) assembled by nanocubes for the first time to realize the objective. The "cocktail effect" of high-entropy construction, rich sodium content of monoclinic phase, and unique hollow structure endow HMHE-HCF cathode with fast reaction kinetics and energetically stable performance during continuous charging/discharging processes. As a result, the HMHE-HCF cathode demonstrates superior rate performance up to an ultra-high rate of 100 C (71.1 % retention to 0.1 C), and remarkable cycling stability with a capacity retention of 77.8 % over 25,000 cycles at 100 C, outperforming most reported sodium-ion cathodes. Further, the HMHE-HCF//hard carbon full-cell delivers capacities of 99.0 and 82.3 mAh g-1 at 0.1 C and 10 C, respectively, and retains 98.1 % of the initial capacity after 1,600 cycles at 5 C, demonstrating its potential application for sodium-ion storage.

Keywords: chemical composition; metal hexacyanoferrates; morphology configuration; sodium ion battery; ultrafast and durable.