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Synergistic Surface Engineering of Zn Anodes through Microwave-Assisted Etching and Polydopamine Coating for Long-Life Aqueous Zinc-Ion Batteries

초록/요약

Aqueous zinc-ion batteries (ZIBs) have emerged as a promising alternative to conventional lithium-ion batteries, owing to their inherent safety, low cost, and high theoretical capacity (820 mA h g-1, 5855 mA h cm-3). However, the commercialization of ZIBs is hindered by their short lifespan, primarily resulting from dendrite growth and parasitic side reactions, such as the hydrogen evolution reaction, corrosion, and byproduct formation on the Zn anode. To address these challenges, ensuring uniform Zn deposition and facilitating the desolvation of hydrated Zn ions at the Zn anode surface are essential. In this work, we propose a surface modification strategy combining microwave-assisted etching with polydopamine (PDA) coating to stabilize the Zn anode and extend the lifespan of ZIBs. Microwave irradiation accelerates the etching reaction, promoting the formation of a porous structure at the Zn surface. Molecular dynamic simulations reveal that the stepped pores exposed at the etched Zn (eZn) surface rapidly adsorb Zn ions and provide numerous nucleation sites for Zn deposition. Furthermore, the PDA coating on the eZn plays a crucial role in mitigating side reactions by capturing H2O molecules from hydrated Zn ions through its abundant polar functional groups. As a result, the developed PDA-coated eZn (PDA-eZn) effectively addresses the major challenges of Zn anodes, demonstrating an excellent lifespan for over 520 h at a current density of 10 mA cm-2 and an areal capacity of 5 mAh cm-2 in symmetric cells. Moreover, a PDA-eZn//V2O5 full cell exhibits a high capacity retention of 73.6% even after 1500 cycles at 3 A g-1.

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목차

Chapter 1. Introduction 1
1.1. Aqueous zinc-ion batteries (ZIBs) 1
1.2. Zn anode with three-dimensional (3D) structure 1
1.3. Protective layer strategies 2
1.4. Synergistic effect of 3D structure and protective layer 3
Chapter 2. Experimental sections 4
2.1. Preparation of PDA-eZn 4
2.2. Assembly of Zn//V2O5 full cells 4
2.3. Assembly of Zn//Cu asymmetric cells 4
2.4. Electrochemical measurements 5
2.5. Computational methods 6
Chapter 3. Results and Discussion 8
3.1. Structural changes of Zn anode by microwave-assisted etching 8
3.2. Confirmation of polydopamine layer formation 13
3.3. Electrochemical cycling performance using Zn//Zn symmetric cells and Zn//Cu asymmetric cells 17
3.4. Dendrite inhibition behavior of stepwise pores 23
3.5. Side reaction suppression properties of PDA 28
3.6. Full cell cycling performance of PDA-eZn 33
Chapter 4. Conclusion 37
Reference 38

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