Key Takeaways & Executive Findings
- •• • Ultrathin PDMS interphase (~5 nm) achieves 2.28-fold enhancement in Zn2+ transference number, enabling rapid ion transport and low polarization, critical for high-rate and high-energy-density batteries. • • The PDMS-modified anode delivers 99.9% Coulombic efficiency over 3500 cycles, indicating exceptional reversibility and minimal side reactions, essential for long-cycle-life energy storage. • • Symmetrical cells operate stably for 880 hours at 60% depth of discharge, demonstrating high Zn utilization and dendrite suppression, which is vital for practical high-energy-density AZIBs. • • Full cells with lean Zn (N/P ratio 5.7) sustain 2500 cycles, and pouch cells with high cathode loading (~7.2 mg cm−2) achieve 1400 cycles with only 0.01% decay rate, proving scalability and commercial viability.
Abstract
Aqueous Zn-ion batteries (AZIBs) are promising for next-generation energy storage due to high safety and low cost, but their practical use is limited by Zn dendrite growth and side reactions. An ideal anode/electrolyte interphase should block water contact while enabling fast Zn2+ transport, yet conventional thick interphases increase ionic resistance and polarization. Here, we report a hydrophobic yet ultrathin (~5 nm) polydimethylsiloxane (PDMS) artificial interphase fabricated via conformal coating. The oxygen-rich PDMS layer selectively coordinates Zn2+ while its superhydrophobicity excludes water, and the ultrathin nature enables rapid Zn2+ conduction, enhancing the Zn2+ transference number by 2.28-fold. This synergistic design suppresses dendrites and mitigates hydrogen evolution. The PDMS-modified anode achieves 99.9% Coulombic efficiency over 3500 cycles, 880-hour symmetrical cell operation at 60% depth of discharge, and 2500-cycle full-cell endurance under lean Zn conditions (N/P ratio 5.7). Proof-of-concept pouch cells sustain 1400 cycles with a 0.01% decay rate. This molecular-scale interphase strategy provides a feasible pathway toward practical AZIB implementation.
1. Introduction
Aqueous Zn-ion batteries (AZIBs) are attractive for grid-scale energy storage due to their inherent safety, low cost, and high theoretical capacity (820 mAh g−1). However, their commercialization is stalled by rampant Zn dendrite growth and corrosive side reactions, which originate from the lack of a durable anode/electrolyte interphase that can regulate ion flux and shield against water erosion. Conventional artificial interphases, such as thick inorganic or organic layers (e.g., 15 μm In2O3, 20–30 μm MOF, 5 μm COF), improve stability but introduce excessive ionic resistance and polarization, particularly for hydrophobic coatings, thereby compromising energy density and rate capability.
This work addresses the bottleneck by constructing an ultrathin (~5 nm) polydimethylsiloxane (PDMS) interphase that combines superhydrophobicity with selective Zn2+ coordination. The molecular-scale thickness minimizes ionic transport barriers, while the elastic PDMS conforms to the anode surface, ensuring crack-free integrity during cycling. This design simultaneously blocks water penetration and facilitates fast Zn2+ conduction, effectively suppressing dendrites and hydrogen evolution. The result is a significant enhancement in cycling stability and Zn utilization, offering a practical pathway for high-performance AZIBs.
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Xinren Zhang, Xu Peng, Zhaodong Wang, Tong Li, Fei Xu (2026). Ultrathin hydrophobic anode/electrolyte interphase for stable zinc-metal anode. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3485-0
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Frequently Asked Questions
What is the failure mechanism of the PDMS interphase under prolonged cycling at high depth of discharge (DOD)?
The PDMS interphase maintains structural integrity for at least 880 hours at 60% DOD in symmetrical cells, indicating excellent resistance to mechanical stress and corrosion. The elastic nature of PDMS accommodates volume changes, preventing cracking and delamination that typically plague rigid inorganic layers. However, beyond this duration, gradual degradation may occur due to cumulative water permeation or electrochemical oxidation, though the study demonstrates unprecedented stability compared to bare Zn anodes.
How does the PDMS interphase achieve selective Zn2+ transport while blocking water, and what is the quantitative impact on transference number?
The oxygen-rich PDMS layer coordinates Zn2+ ions preferentially over water molecules due to favorable interactions, while its superhydrophobicity repels water. This selective transport enhances the Zn2+ transference number by 2.28-fold, reducing concentration polarization and promoting uniform deposition. The ultrathin (~5 nm) thickness minimizes ionic resistance, enabling rapid Zn2+ conduction without compromising the hydrophobic barrier.
What are the scalability and cost implications of the PDMS coating process for commercial AZIB production?
PDMS is a low-cost, industrially available polymer, and the conformal coating method (likely spin-coating or dip-coating) is compatible with roll-to-roll manufacturing. The ultrathin layer requires minimal material, reducing cost. The demonstrated performance in pouch cells with high cathode loading (~7.2 mg cm−2) and 1400 cycles indicates scalability. However, precise thickness control and uniformity over large areas must be validated for mass production.
How does the PDMS interphase affect the energy density of full cells compared to bare Zn anodes?
The ultrathin PDMS layer adds negligible mass and volume, preserving the theoretical energy density of the Zn anode. By enabling high Zn utilization (60% DOD) and stable cycling under lean Zn conditions (N/P ratio 5.7), the effective energy density is significantly improved compared to bare Zn, which typically operates at DOD <10% to avoid dendrites. The 2500-cycle full-cell endurance demonstrates that the interphase does not compromise capacity retention.
What is the role of the oxygen groups in the PDMS interphase for Zn2+ coordination, and how does it influence deposition morphology?
The oxygen-containing functional groups (e.g., Si-O-Si) in PDMS act as coordination sites for Zn2+, facilitating desolvation and uniform nucleation. This selective coordination homogenizes the Zn2+ flux, as confirmed by in-situ optical microscopy, leading to dendrite-free deposition. The superhydrophobic nature excludes water, minimizing hydrogen evolution and byproduct formation, which further stabilizes the anode-electrolyte interface.
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