Reversible K-Ion intercalation in CrSe2 cathodes for potassium-ion batteries: Combined operando PXRD and DFT studies

In the pursuit of more affordable battery technologies, potassium-ion batteries (KIBs) have emerged as a promising alternative to lithium-ion systems, owing to the abundance and wide distribution of potassium resources. While chalcogenides are uncommon as intercalation cathodes in KIBs, this study's electrochemical tests on CrSe2 revealed a reversible K+ ion intercalation/deintercalation process. The CrSe2 cathode achieved a KIB battery capacity of 125 mAh/g at a 0.1C rate within a practical 1- 3.5 V vs K+/K operation range, nearly matching the theoretical capacity of 127.7 mAh/g. Notably, the battery retained 85% of its initial capacity at a high 1C rate, suggesting that CrSe2 is competitive for high-power applications with many current state-of-the-art cathodes. In-operando PXRD studies uncovered the nature of the intercalation behavior, revealing an initial biphasic region followed by a solid-solution formation during the potassium intercalation process. DFT calculations helped with the possible assignment of intermediate phase structures across the entire CrSe2 – K1.0CrSe2 composition range, providing insights into the experimentally observed phase transformations. The results of this work underscore CrSe2's potential as a high-performance cathode material for KIBs, offering valuable insights into the intercalation mechanisms of layered transition metal chalcogenides and paving the way for future advancements in optimizing KIB cathodes