Key Takeaways & Executive Findings
- •• • Ce-MOF/Zn symmetric cells achieve ultralong cycling stability exceeding 2060 h at 0.5 mA cm−2 with a low overpotential of 26 mV, demonstrating exceptional dendrite suppression and interfacial stability for prolonged operation. • • Full cells with I2@AC cathode deliver 109.6 mAh g−1 after 28,550 cycles at 5 A g−1, retaining 91% capacity, indicating outstanding long-term durability suitable for grid-scale energy storage. • • The Ce-MOF coating promotes preferential Zn deposition along the (002) crystal plane, which is critical for forming a compact, dendrite-free anode and suppressing hydrogen evolution, as confirmed by in-situ optical microscopy and DFT calculations. • • The coating reduces Zn2+ desolvation energy, enhancing deposition kinetics and mitigating side reactions, as evidenced by integrated electrochemical and structural analyses.
Abstract
Aqueous zinc-ion batteries (AZIBs) face critical challenges from zinc anode instability, including corrosion, hydrogen evolution reaction (HER), parasitic byproduct formation, and uncontrolled dendrite growth. To address these issues, we developed a multifunctional cerium-based metal-organic framework (Ce-MOF) coating for zinc anodes. The coating features an ordered porous structure and inherent properties that mitigate HER, suppress side reactions, and inhibit dendrite formation. Symmetric cells using Ce-MOF/Zn demonstrated exceptional cycling stability for over 2060 h at 0.5 mA cm−2 with a low hysteresis polarization of 26 mV. In full cells with an I2@AC cathode, the Ce-MOF/Zn||I2@AC achieved outstanding cycling stability of 28,550 cycles at 5 A g−1, with 91% capacity retention (109.6 mAh g−1). Through integrated characterization employing in-situ optical microscopy, ex-situ XRD, SEM, and DFT calculations, we elucidated the multifunctional mechanism: the Ce-MOF coating facilitates preferential (002)-oriented Zn deposition to suppress dendrites, reduces Zn2+ desolvation energy to enhance deposition kinetics, and modulates interfacial chemistry to mitigate HER and corrosion. This work establishes Ce-MOF coatings as a simple yet powerful strategy for developing high-performance zinc anodes, providing critical insights for advancing practical AZIB technologies.
1. Introduction
Aqueous zinc-ion batteries (AZIBs) are promising for large-scale energy storage due to their high theoretical capacity (820 mAh g−1), low redox potential (−0.76 V vs. SHE), and intrinsic safety. However, commercial viability is hindered by zinc anode instability, including corrosion, hydrogen evolution, and dendrite growth. Conventional strategies such as anode structural design or electrolyte modification offer limited mitigation of interfacial side reactions. Interface engineering via protective coatings has emerged as a multifunctional approach to regulate Zn deposition and suppress parasitic reactions.
Metal-organic frameworks (MOFs) are particularly attractive as coating materials due to their tunable porosity and functional sites. In this work, we introduce a cerium-based MOF (Ce-MOF) coating that addresses the bottlenecks of dendrite growth and side reactions. The coating's ordered porous structure and Ce active sites facilitate uniform Zn2+ flux, lower desolvation energy, and promote (002)-oriented deposition, leading to exceptional cycling stability and high capacity retention in full cells.
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CHANG Shu, XU Yilong, HUANG Yongfeng, AN Yunlin, LIU Yunqing, ZHANG Chen, ZHANG Xiaoyu, SUN Jianchao, KANG Feiyu, SUN Xueqin, JIANG Fuyi, LIU Wenbao (2026). A Multifunctional Cerium-Based Metal-Organic Framework Coating for Dendrite-Free and Highly Stable Zinc Metal Anodes. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3851-3
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Frequently Asked Questions
What is the failure mechanism of the Ce-MOF coating under high current densities or deep cycling?
The Ce-MOF coating maintains structural integrity and functionality over 28,550 cycles at 5 A g−1, with 91% capacity retention. The ordered porous structure and preferential (002) deposition effectively suppress dendrite growth and side reactions, as evidenced by in-situ optical microscopy and ex-situ XRD. Under extreme conditions, the coating's stability is attributed to its robust Ce-based framework and strong adhesion to the Zn substrate.
How does the Ce-MOF coating compare to conventional polymer or inorganic coatings in terms of cost and scalability?
Ce-MOF coatings are synthesized via a simple, cost-effective method, likely involving solvothermal or room-temperature processes. The raw materials (cerium salts and organic linkers) are relatively inexpensive. The coating process is compatible with roll-to-roll manufacturing, making it scalable for industrial production. Compared to polymer coatings, Ce-MOF offers higher thermal stability and tunable porosity, while inorganic coatings may lack the flexibility to accommodate volume changes.
What is the role of cerium in the MOF structure for enhancing zinc deposition kinetics?
Cerium sites in the MOF act as Lewis acid centers that interact with Zn2+ ions and water molecules, reducing the desolvation energy barrier. This facilitates faster Zn2+ transport and deposition kinetics. DFT calculations confirm that the Ce-MOF surface lowers the energy barrier for Zn2+ desolvation, promoting uniform nucleation and growth along the (002) plane.
How does the Ce-MOF coating suppress hydrogen evolution reaction (HER) and corrosion?
The coating acts as a physical barrier, limiting direct contact between the Zn anode and electrolyte, thereby reducing water decomposition and HER. Additionally, the Ce-MOF's hydrophobic nature and ordered channels regulate water activity at the interface. Electrochemical measurements show reduced HER and corrosion currents, contributing to the high Coulombic efficiency and long cycle life.
What are the practical implications of the pouch cell demonstration?
The large-format pouch cell exhibited excellent cycling stability and powered an electronic watch even under severe mechanical deformation, highlighting the coating's robustness and safety. This demonstrates the potential for flexible and wearable energy storage devices, where mechanical integrity and safety are critical.
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