Phase Evolution of Multi‐Metal Dichalcogenides With Conversion‐Alloying Hybrid Mechanism for Superior Lithium Storage

Authors: Jingjing Jiang, Sanlue Hu, Xiangyong Zhang, Senlin Li, Hua Wei, Baohui Ren, Shizhen Li, Guangming Chen, Jinlong Yang, Cuiping Han, Zhuoxin Liu

Published: 2024-05-04

DOI: 10.1002/adma.202311926

Source: Full article


Abstract

AbstractTraditional lithium‐ion battery (LIB) anodes, whether intercalation‐type like graphite or alloying‐type like silicon, employing a single lithium storage mechanism, are often limited by modest capacity or substantial volume changes. Here, the kesterite multi‐metal dichalcogenide (CZTSSe) is introduced as an anode material that harnesses a conversion‐alloying hybrid lithium storage mechanism. Results unveil that during the charge–discharge processes, the CZTSSe undergoes a comprehensive phase evolution, transitioning from kesterite structure to multiple dominant phases of sulfides, selenides, metals, and alloys. The involvement of multi‐components facilitates electron transport and mitigates swelling stress; meanwhile, it results in formation of abundant defects and heterojunctions, allowing for increased lithium storage active sites and reduced lithium diffusion barrier. The CZTSSe delivers a high specific capacity of up to 2266 mA h g−1 at 0.1 A g−1; while, maintaining a stable output of 116 mA h g−1 after 10 000 cycles at 20 A g−1. It also demonstrates remarkable low‐temperature performance, retaining 987 mA h g−1 even after 600 cycles at −40 °C. When employed in full cells, a high specific energy of 562 Wh kg−1 is achieved, rivalling many state‐of‐the‐art LIBs. This research offers valuable insights into the design of LIB electrodes leveraging multiple lithium storage mechanisms.