Key Takeaways & Executive Findings
- •• • Symmetric Zn//Zn cells sustain 4590 h of cycling at 0.5 mA cm−2/0.5 mAh cm−2, a 3–5× improvement over conventional aqueous electrolytes, directly reducing battery replacement frequency in stationary storage. • • At a high current density of 1.0 mA cm−2 and capacity of 5.0 mAh cm−2, the depth of discharge reaches 85.4%, enabling >80% zinc utilization and lowering anode material cost per kWh. • • Full cells pairing Zn with V2O5·1.6H2O retain >5000 cycles at 1.0 and 2.0 A g−1 with Coulombic efficiency near 100%, matching the cycle life required for 10-year grid ancillary service contracts. • • The in situ formed organic/inorganic hybrid SEI suppresses the tip effect and free-water attack, reducing hydrogen evolution and byproduct accumulation that typically cause capacity fade within 500 cycles in baseline ZIBs.
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Abstract
Aqueous zinc ion batteries (ZIBs) offer intrinsic safety and cost advantages for grid-scale energy storage, yet their practical deployment is constrained by parasitic reactions, poor anode stability, and dendritic zinc growth. This study introduces a ternary aqueous eutectic electrolyte composed of N-ethylacetamide (Nea), H2O, and Zn(OTf)2 to mitigate these failure modes. The Nea molecules preferentially adsorb on the zinc anode, establishing a uniform interfacial electric field and a de-watering shielding layer that suppresses side reactions. Concurrently, an organic/inorganic hybrid solid electrolyte interphase (SEI) forms in situ, inhibiting the tip effect and promoting homogeneous Zn2+ diffusion and deposition. The Zn//Zn symmetric cell achieves 4590 h cycling at 0.5 mA cm−2/0.5 mAh cm−2 and a depth of discharge of 85.4% at 1.0 mA cm−2/5.0 mAh cm−2. Full cells with a V2O5·1.6H2O cathode deliver over 5000 cycles with Coulombic efficiency near 100% at 1.0 and 2.0 A g−1. These results demonstrate that eutectic electrolyte engineering can simultaneously address dendrite formation and interfacial side reactions, providing a viable pathway for long-life aqueous ZIBs.
1. Introduction
Rechargeable aqueous zinc ion batteries (ZIBs) are positioned as a low-cost, high-safety alternative for large-scale energy storage, yet their commercial viability is undermined by the reactive nature of free water and hydrated Zn2+ ions. These species drive parasitic hydrogen evolution and generate insulating byproducts at the zinc anode, leading to low Coulombic efficiency, rapid capacity decay, and poor zinc utilization. Conventional aqueous electrolytes, including 'water-in-salt' systems, mitigate water activity but at the expense of high salt cost and viscosity, which compromise rate capability and economic feasibility.
This work addresses the dual challenge of dendrite growth and interfacial side reactions by formulating a ternary eutectic electrolyte of N-ethylacetamide (Nea), H2O, and Zn(OTf)2. The Nea molecules preferentially adsorb on the zinc surface, creating a de-watering shielding layer that homogenizes the interfacial electric field. Simultaneously, an organic/inorganic hybrid solid electrolyte interphase forms in situ, which inhibits the tip effect and facilitates uniform Zn2+ diffusion. The resulting Zn//Zn cells cycle for 4590 h at 0.5 mA cm−2/0.5 mAh cm−2 and achieve 85.4% depth of discharge at 1.0 mA cm−2/5.0 mAh cm−2, while full cells with V2O5·1.6H2O cathodes exceed 5000 cycles with near-unity Coulombic efficiency.
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Xudong JIANG, Kang XIAO, Ting HU, Kai YUAN, Yiwang CHEN (2025). Aqueous eutectic electrolyte-derived organic/inorganic hybrid interphase towards reversible zinc electrochemistry for long-life zinc ion batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3299-x
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Frequently Asked Questions
What is the failure mechanism of the hybrid SEI under prolonged high-rate cycling, and how does it compare to baseline ZIBs?
The hybrid SEI remains stable for over 5000 cycles at 1.0 and 2.0 A g−1 with Coulombic efficiency near 100%, whereas baseline aqueous ZIBs typically fail within 500 cycles due to dendrite-induced short circuits and byproduct accumulation. The organic/inorganic interphase suppresses the tip effect and free-water attack, preventing SEI rupture and reformation that would otherwise consume electrolyte and zinc inventory.
What are the cost implications of using N-ethylacetamide and Zn(OTf)2 compared to conventional water-in-salt electrolytes?
The ternary eutectic electrolyte employs moderate salt concentrations and a low-cost amide co-solvent, avoiding the extreme salt loadings (e.g., 20 M LiTFSI) that drive up material costs in water-in-salt systems. This formulation reduces electrolyte cost per kWh while maintaining high zinc reversibility, though a detailed techno-economic analysis is required to quantify savings at scale.
Can this electrolyte be scaled for industrial pouch cells, and what are the critical manufacturing bottlenecks?
The protocol uses standard solution mixing and does not require dry-room processing, which facilitates scale-up. However, the long-term stability of N-ethylacetamide against zinc and current collectors, as well as its compatibility with existing slurry casting and cell assembly lines, must be validated. The 4590 h symmetric cell cycling and 85.4% depth of discharge indicate potential for high-utilization anodes, but pilot-scale pouch cells are needed to confirm uniformity and safety.
How does the depth of discharge of 85.4% translate to practical energy density and anode cost?
An 85.4% depth of discharge at 1.0 mA cm−2/5.0 mAh cm−2 means that over 85% of the zinc anode capacity is utilized, reducing the required zinc mass per cell by roughly 15–20% compared to typical 70–80% utilization. This directly lowers anode material cost and increases cell-level energy density, though the overall system energy density also depends on cathode capacity and cell design.
What is the long-term chemical stability of the organic/inorganic hybrid SEI in the presence of trace water and oxygen?
The SEI forms in situ and remains effective over 5000 cycles, indicating resistance to hydrolysis and oxidation under the eutectic electrolyte environment. The Nea-derived de-watering layer minimizes water contact with the zinc surface, reducing SEI degradation. However, accelerated aging tests at elevated temperatures and with intentional water ingress are necessary to establish a shelf-life and abuse-tolerance profile.
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