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Angewandte Chemie International Edition, 2021-05, Vol.60 (20), p.11481-11486
Auflage
International ed. in English
Ort / Verlag
Germany: Wiley Subscription Services, Inc
Erscheinungsjahr
2021
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
High initial coulombic efficiency is highly desired because it implies effective interface construction and few electrolyte consumption, indicating enhanced batteries’ life and power output. In this work, a high‐capacity sodium storage material with FeS2 nanoclusters (≈1–2 nm) embedded in N, S‐doped carbon matrix (FeS2/N,S‐C) was synthesized, the surface of which displays defects‐repaired characteristic and detectable dot‐matrix distributed Fe‐N‐C/Fe‐S‐C bonds. After the initial discharging process, the uniform ultra‐thin NaF‐rich (≈6.0 nm) solid electrolyte interphase was obtained, thereby achieving verifiable ultra‐high initial coulombic efficiency (≈92 %). The defects‐repaired surface provides perfect platform, and the catalysis of dot‐matrix distributed Fe‐N‐C/Fe‐S‐C bonds to the rapid decomposing of NaSO3CF3 and diethylene glycol dimethyl ether successfully accelerate the building of two‐dimensional ultra‐thin solid electrolyte interphase. DFT calculations further confirmed the catalysis mechanism. As a result, the constructed FeS2/N,S‐C provides high reversible capacity (749.6 mAh g−1 at 0.1 A g−1) and outstanding cycle stability (92.7 %, 10 000 cycles, 10.0 A g−1). Especially, at −15 °C, it also obtains a reversible capacity of 211.7 mAh g−1 at 10.0 A g−1. Assembled pouch‐type cell performs potential application. The insight in this work provides a bright way to interface design for performance improvement in batteries.
A defect‐repairing‐induced dot–matrix distributed interface efficiently catalyzes electrolyte decomposition. This strategy enables an ultra‐thin and robust solid–electrolyte interface achieving ultra‐high initial coulombic efficiency in sodium‐ion batteries.