Interfacial optimization enabling reversible and stable aqueous zinc metal batteries under harsh conditions

Abstract

Aqueous zinc metal batteries (AZMBs) have garnered widespread attention due to their low cost and high safety. However, current researches are still primarily focused on reversible cycling at low areal capacity, which is far from practical application. Addressing interfacial stability issues encountered during cycling and employing interfacial optimization strategies can promote the development of safe and eco-friendly AZMBs. By introducing γ-valerolactone (GVL), which disrupts the original hydrogen bonding network of water, the electrochemical window of electrolyte is expanded, and the reactivity of water is significantly reduced. Additionally, the incorporation of GVL in Zn ion solvation alters the deposition pattern on the Zn anode surface, resulting in improved cyclic performance. The cells demonstrated excellent performance, maintaining stable over 400 h at 5 mA/cm²-5 mA·h/cm², and nearly 300 h in Zn∥Zn symmetric cell at 80% depth of discharge (DOD). The full cells matched with NH₄V₄O₁₀ could cycle over 200 cycles under the condition of high areal capacity (7 mA·h/cm²), an N/P ratio of 1.99 and an E/C ratio of 9.3 µL/(mA·h).

References

[1] Liu Z-x, Li L-y, Qin L-p, et al.. Balanced interfacial ion concentration and migration steric hindrance promoting high-efficiency deposition/dissolution battery chemistry [J]. Advanced Materials, 2022, 34(40): e2204681.

[2] Cui Y, Ding Y, Guo L-f, et al.. Ultra-long Zn₃V₂O₇(OH)₂·2H₂O nanowires grown on carbon cloth as cathode material for aqueous zinc-ion batteries [J]. Energy Materials, 2023, 3: 300023

[3] Wang Z-q, Zhou M, Qin L-p, et al.. Simultaneous regulation of cations and anions in an electrolyte for high-capacity, high-stability aqueous zinc-vanadium batteries [J]. eScience, 2022, 2(2): 209-218.

[4] Lin Y-x, Mai Z-x, Liang H-k, et al.. Dendrite-free Zn anode enabled by anionic surfactant-induced horizontal growth for highly-stable aqueous Zn-ion pouch cells [J]. Energy & Environmental Science, 2023, 16(2): 687-697.

[5] Li H-f, Ma L-t, Han C-p, et al.. Advanced rechargeable zinc-based batteries: Recent progress and future perspectives [J]. Nano Energy, 2019, 62: 550-587.

[6] Qin H-y, Kuang W, Hu N, et al.. Building metal-molecule interface towards stable and reversible Zn metal anodes for aqueous rechargeable zinc batteries [J]. Advanced Functional Materials, 2022, 32(47): 2206695.

[7] Chen J-z, Zhou W-j, Quan Y-h, et al.. Ionic liquid additive enabling anti-freezing aqueous electrolyte and dendrite-free Zn metal electrode with organic/inorganic hybrid solid electrolyte interphase layer [J]. Energy Storage Materials, 2022, 53: 629-637.

[8] Zhu J-l, Deng W-j, Yang N, et al.. Biomolecular regulation of zinc deposition to achieve ultra-long life and high-rate Zn metal anodes [J]. Small, 2022, 18(29): e2202509.

[9] Chen Y, Tan X-p, Fang G-z, et al.. Electrochemical basis and regulation of electrode materials for secondary batteries [J]. The Chinese Journal of Nonferrous Metals, 2021, 31(11): 3232-3253 (in Chinese)

[10] Dou X-y, Xie X-f, Liang S-q, et al.. Low-current-density stability of vanadium-based cathodes for aqueous zinc-ion batteries [J]. Science Bulletin, 2024, 69(6): 833-845.

[11] Guo S, Qin L-p, Wu J, et al.. Conversion-type anode chemistry with interfacial compatibility toward Ah-level near-neutral high-voltage zinc ion batteries [J]. National Science Review, 2024, 11(7): nwae181.

[12] Huang J, Peng Q, Liu K, et al.. Silica-based electrolyte regulation for stable aqueous zinc-manganese batteries [J]. Journal of Central South University, 2023, 30(2): 434-442.

[13] Miao L-c, Guo Z-p, Jiao L-fang. Insights into the design of mildly acidic aqueous electrolytes for improved stability of Zn anode performance in zinc-ion batteries [J]. Energy Materials, 2023, 3: 300014

[14] Xie K-x, Ren K-x, Wang Q-h, et al.. In situ construction of zinc-rich polymeric solid-electrolyte interface for high-performance zinc anode [J]. eScience, 2023, 3(4): 100153.

[15] Zou P-c, Lin R-q, Pollard T P, et al.. Localized hydrophobicity in aqueous zinc electrolytes improves zinc metal reversibility [J]. Nano Letters, 2022, 22(18): 7535-7544.

[16] Huang Z-c, Li H-y, Yang Z, et al.. Nanosecond laser lithography enables concave-convex zinc metal battery anodes with ultrahigh areal capacity [J]. Energy Storage Materials, 2022, 51: 273-285.

[17] Wang R, Wu L-y, Wei Y, et al.. ‘Two birds with one stone’ design for dendrite-free zinc-metal anodes: Three-dimensional highly conductive skeletons loaded with abundant zincophilic sites [J]. Materials Today Energy, 2022, 29: 101097.

[18] Li C, Jin S, Archer L A, et al.. Toward practical aqueous zinc-ion batteries for electrochemical energy storage [J]. Joule, 2022, 6(8): 1733-1738.

[19] Yang S-n, Du H-x, Li Y-t, et al.. Advances in the structure design of substrate materials for zinc anode of aqueous zinc ion batteries [J]. Green Energy & Environment, 2023, 8(6): 1531-1552.

[20] Niu B, Li Z-g, Luo D, et al.. Nano-scaled hydrophobic confinement of aqueous electrolyte by a nonionic amphiphilic polymer for long-lasting and wide-temperature Zn-based energy storage [J]. Energy & Environmental Science, 2023, 16(4): 1662-1675.

[21] Yang F-h, Yuwono J A, Hao J-n, et al.. Understanding H₂ evolution electrochemistry to minimize solvated water impact on zinc-anode performance [J]. Advanced Materials, 2022, 34(45): 2206754.

[22] Zhao H-n, Fu Q, Luo X-l, et al.. Unraveling a cathode/anode compatible electrolyte for high-performance aqueous rechargeable zinc batteries [J]. Energy Storage Materials, 2022, 50: 464-472.

[23] Wu C-p, Sun C, Ren K-x, et al.. 2-methyl imidazole electrolyte additive enabling ultra-stable Zn anode [J]. Chemical Engineering Journal, 2023, 452: 139465.

[24] Wang N, Dong X-l, Wang B-l, et al.. Zinc-organic battery with a wide operation-temperature window from - 70 to 150 °C [J]. Angewandte Chemie International Edition, 2020, 59(34): 14577-14583.

[25] Peng M-k, Tang X-n, Xiao K, et al.. Polycation-regulated electrolyte and interfacial electric fields for stable zinc metal batteries [J]. Angewandte Chemie (International Ed), 2023, 62(27): e202302701.

[26] Qin Y, Li H-f, Han C-p, et al.. Chemical welding of the electrode - electrolyte interface by Zn-metal-initiated in situ gelation for ultralong-life Zn-ion batteries [J]. Advanced Materials, 2022, 34(44): 2207118.

[27] Bie Z, Yang Q, Cai X-x, et al.. One-step construction of a polyporous and zincophilic interface for stable zinc metal anodes [J]. Advanced Energy Materials, 2022, 12(44): 2202683.

[28] Tang B-y, Zhou J, Fang G-z, et al.. Engineering the interplanar spacing of ammonium vanadates as a high-performance aqueous zinc-ion battery cathode [J]. Journal of Materials Chemistry A, 2019, 7(3): 940-945.

[29] Hu Y-d, Liu Z-x, Li L-y, et al.. Reconstructing interfacial manganese deposition for durable aqueous zinc-manganese batteries [J]. National Science Review, 2023, 10(10): nwad220.

[30] Yang X, Zhang Z-y, Wu M-l, et al.. Reshaping zinc plating/stripping behavior by interfacial water bonding for high-utilization-rate zinc batteries [J]. Advanced Materials, 2023, 35(49): e2303550.

[31] Shen Z-y, Mao J-l, Yu G-p, et al.. Electrocrystallization regulation enabled stacked hexagonal platelet growth toward highly reversible zinc anodes [J]. Angewandte Chemie (International Ed), 2023, 62(11): e202218452.

[32] Li G-j, Zhao Z-h, Zhang S-l, et al.. A biocompatible electrolyte enables highly reversible Zn anode for zinc ion battery [J]. Nature Communications, 2023, 14(1): 6526.

[33] Li C, Kingsbury R, Thind A S, et al.. Enabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries [J]. Nature Communications, 2023, 14(1): 3067.

[34] Wang Y-y, Wang Z-j, Pang Wei k, et al.. Solvent control of water O—H bonds for highly reversible zinc ion batteries [J]. Nature Communications, 2023, 14(1): 2720.

RIGHTS & PERMISSIONS

Central South University