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batteries Review An Overview of Challenges and Strategies for Stabilizing Zinc Anodes in Aqueous Rechargeable Zn-Ion Batteries Nhat Anh Thieu 1, Wei Li 1,* , Xiujuan Chen 1, Shanshan Hu 1 , Hanchen Tian 1, Ha Ngoc Ngan Tran 2, Wenyuan Li 2, David M. Reed 3, Xiaolin Li 3,* and Xingbo Liu 1,* 1 2 3 Abstract: Aqueous rechargeable zinc ion batteries (ZIBs) have been revived and are considered a promising candidate for scalable electrochemical energy storage systems due to their intrinsic safety, low cost, large abundance, mature recyclability, competitive electrochemical performance, and sustainability. However, the deployment of aqueous rechargeable ZIBs is still hampered by the poor electrochemical stability and reversibility of Zn anodes, which is a common, inherent issue for most metal-based anodes. This review presents a comprehensive and timely overview of the challenges and strategies of Zn anodes toward durable ZIBs. First, several challenges that significantly reduce the Coulombic efficiency and cycling stability of Zn anodes are briefly discussed including dendrite formation, hydrogen evolution, and corrosion. Then, the mitigation strategies are summarized in terms of modifying the electrode/electrolyte interfaces, designing electrode structures, and optimizing electrolytes and separators. Further, we comprehensively discuss the mechanisms behind these issues and improvement strategies with respect to the anodes, electrolytes, and separators. Lastly, we provide perspectives and critical analyses of remaining challenges, outlook, and future direction for accelerating the practical application of aqueous rechargeable ZIBs. Keywords: zinc ion batteries; Zn metal anode; dendrite; corrosion; hydrogen evolution 1. Introduction Electrochemical energy storage systems that can store energy from green and renew- able sources are essential for reducing electricity overconsumption and environmental pollution. Among various forms of electrical energy storage, batteries store energy as chemical potential in the electrodes via redox reactions. One well-known example is the prevailing lithium-ion batteries (LIBs), which have a high energy density, superior cycle life, and low weight making them ideal for powering portable electronics and electric vehicles. Unfortunately, the application of LIBs in grid energy systems is hindered by the potential risk and environmental concerns occurring from highly reactive lithium compounds and flammable organic electrolytes [1–6]. The most significant safety concern associated with LIBs is a thermal runaway, which results in battery rupture and explosion as flammable gases from the battery react with ambient oxygen [7,8]. There are several origins of thermal runaway in batteries, including side reactions involving organic electrolytes, cathodes, and anodes, and interactions between electrode surfaces and Li plating caused by thermal, electrical, and thermal abuse without effective battery management and risk monitoring [9]. Moreover, LIBs often experience different types of improper operation during daily usage, such as overcharging and over-discharging due to variations in cell capacities caused by manufacturing processes, over-heating enabled by poor battery system temperature man- agement, elevated ambient temperature or nearby fire, and physical damage impact [10]. Department of Mechanical and Aerospace Engineering, Benjamin M. Statler College of Engineering and Mineral Resources, West Virginia University, Morgantown, WV 26506, USA Department of Chemical and Biomedical Engineering, Benjamin M. Statler College of Engineering and Mineral Resources, West Virginia University, Morgantown, WV 26506, USA Pacific Northwest National Laboratory, Richland, WA 99354, USA * Correspondence: wei.li@mail.wvu.edu (W.L.); xiaolin.li@pnnl.gov (X.L.); xingbo.liu@mail.wvu.edu (X.L.) Citation: Thieu, N.A.; Li, W.; Chen, X.; Hu, S.; Tian, H.; Tran, H.N.N.; Li, W.; Reed, D.M.; Li, X.; Liu, X. An Overview of Challenges and Strategies for Stabilizing Zinc Anodes in Aqueous Rechargeable Zn-Ion Batteries. Batteries 2023, 9, 41. https://doi.org/10.3390/ batteries9010041 Academic Editor: Matthieu Dubarry Received: 28 November 2022 Revised: 26 December 2022 Accepted: 27 December 2022 Published: 5 January 2023 Copyright: © 2023 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ 4.0/). Batteries 2023, 9, 41. https://doi.org/10.3390/batteries9010041 https://www.mdpi.com/journal/batteriesPDF Image | Zinc Anodes in Aqueous Rechargeable Zn-Ion Batteries
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