Electric Double Layer Oriented Eutectic Additive Design toward Stable Zn Anodes with a High Depth of Discharge

Huida Lyu; Siwei Zhao; Chenyi Liao; Guohui Li; Jian Zhi; Fuqiang Huang

doi:10.1002/adma.202400976

Electric Double Layer Oriented Eutectic Additive Design toward Stable Zn Anodes with a High Depth of Discharge

Adv Mater. 2024 May 13:e2400976. doi: 10.1002/adma.202400976. Online ahead of print.

Authors

Huida Lyu^{1

2}, Siwei Zhao^{1

2}, Chenyi Liao³, Guohui Li³, Jian Zhi⁴, Fuqiang Huang^{1

2

5}

Affiliations

¹ School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
² College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
³ Laboratory of Molecular Modeling and Design, State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023, P. R. China.
⁴ CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P. R. China.
⁵ Zhongke Institute of Strategic Emerging Materials, Yixing, Jiangsu, 214213, China.

PMID: 38740388
DOI: 10.1002/adma.202400976

Abstract

ZnSO₄-based electrolytes for aqueous zinc ion batteries fail to meet practical application metrics due to hydrogen evolution reaction (HER) and dendrite growth. In this work, a highly polarized eutectic additive, glycerophosphorylcholine (GPC) is rationally designed, to regulate the electric double layer (EDL) structure for stable Zn anodes with a high depth of discharge (DOD). On one hand, GPC molecules with abundant hydroxyl groups can precisely regulate the hydrogen bond network in EDL to suppress HER. On the other hand, the enrichment of GPC at the interface is positively responsible for the negative charge density on the Zn surface, which leads to the formation of a robust Zn_xP_yO_z-rich solid-electrolyte interphase and terminates dendrite growth in the charge-rich sites. This EDL-oriented eutectic additive engineering enables highly reversible and selectively (002)-textured Zn anodes to operate for over 1450 h at a high DOD of 45.3%. Meanwhile, a high-capacity (185.7 mAh g^-1) aqueous Zn||VS₂ full cell shows remarkable cycling stability over 220 cycles with an excellent capacity retention of 90.4% even at a low current density of 0.1 A g^-1 (0.5 C). This work sheds light on electrolyte design and interface engineering for high-performance aqueous batteries.

Keywords: Zn anodes; aqueous zinc ion batteries; depth of discharge; electric double layer; eutectic.

Abstract

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