Manipulating Electric Double Layer Adsorption for Stable Solid-Electrolyte Interphase in 2.3 Ah Zn-Pouch Cells

作者：Wang, Yu; Liang, Bochun; Zhu, Jiaxiong; Li, Geng; Li, Qing; Ye, Ruquan; Fan, Jun^*; Zhi, Chunyi^*

来源：Angewandte Chemie - International Edition, 2023, 62(23): e202302583.

DOI：10.1002/anie.202302583

• Bulk Solvation
• Crown Ether
• Electric Double Layer
• Pouch Cell
• Zn Anode

Constructing a reliable solid-electrolyte interphase (SEI) is imperative for enabling highly reversible zinc metal (Zn-0) electrodes. Contrary to conventional "bulk solvation" mechanism, we found the SEI structure is dominated by electric double layer (EDL) adsorption. We manipulate the EDL adsorption and Zn2+ solvation with ether additives (i.e. 15-crown-5, 12-crown-4, and triglyme). The 12-crown-4 with medium adsorption on EDL leads to a layer-structured SEI with inner inorganic ZnFx/ZnSx and outer organic C-O-C components. This structure endows SEI with high rigidness and strong toughness enabling the 100 cm(2) Znj jZn pouch cell to exhibit a cumulative capacity of 4250 mAh cm(-2) at areal-capacity of 10 mAh cm(-2). More importantly, a 2.3 Ah Zn vertical bar broken vertical bar Zn0.25V2O5 center dot nH(2)O pouch cell delivers a recorded energy density of 104 WhL(cell)(-) and runs for > 70 days under the harsh conditions of low negative/positive electrode ratio (2.2 : 1), lean electrolyte (8 gAh(-1)), and high-areal-capacity (approximate to 13 mAh cm(-2)).