High-Entropy Prussian Blue Analogues and Their Oxide Family as Sulfur Hosts for Lithium-Sulfur Batteries

Angew Chem Int Ed Engl. 2022 Oct 10;61(41):e202209350. doi: 10.1002/anie.202209350. Epub 2022 Sep 8.

Abstract

The introduction of high-entropy into Prussian blue analogues (PBAs) has yet to attract attention in the field of lithium-sulfur battery materials. Herein, we systematically synthesize a library of PBAs from binary to high-entropy by a facile coprecipitation method. The coordination environment in PBAs is explored by X-ray absorption fine structure spectroscopy, which together with elemental mapping confirm the successful introduction of all metals. Importantly, electrochemical tests demonstrate that high-entropy PBA can serve as polysulfide immobilizer to inhibit shuttle effect and as catalyst to promote polysulfides conversion, thereby boosting its outstanding performance. Additionally, a variety of nanocubic metal oxides from binary to senary are fabricated by using PBAs as sacrificial precursors. We believe that a wide range of new materials obtained from our coprecipitation and pyrolysis methodology can promote further developments in research on PBA systems and sulfur hosts.

Keywords: Catalyst; High-Entropy; Lithium-Sulfur Batteries; Polysulfide Immobilizer; Prussian Blue Analogues.