Zinc batteries were invented in the eighteenth century, but are still in widespread use as primary commercial batteries known as aqueous alkaline batteries. In this article, we discuss the state of the art of rechargeable aqueous zinc batteries. On the one side of the battery cell, porous zinc metal electrodes offer high energy and power densities. On the other side, zinc‐air batteries perform oxygen electrocatalysis in air electrodes, while zinc‐ion batteries use intercalation electrodes. These electrodes are connected by aqueous alkaline or aqueous neutral electrolytes. We introduce the basic history, concepts, and challenges of each technology. Our overview is spiced with some details of current research.
Next-generation batteries strive for the optimal fit in performance, cost, and environmental safety. Within recent times, a whole playground of different material systems and working principles were investigated. Consumer alkaline batteries with a metallic zinc anode and manganese dioxide cathode achieve excellent energy densities of [1], yet their development stalled due to their limited rechargeability. Switching the aqueous electrolyte from alkaline KOH to, for example, mild electrolytes, however, showed a reversible charge/discharge mechanism at the cathode [2]. This achievement highly increased the research interest in zinc-ion batteries in the last decade, and many successful systems were proposed [3], [4]. Aqueous metal batteries face a series of challenges. The limited stability window of water, as well as unwanted precipitation reactions, deteriorate the battery performance and increase aging reactions. The electrolytes composition and the concentration-dependent complex formation governs its performance. Within Zinc-air batteries, we performed model-based optimization studies of pH adjusted electrolytes [5]. Yet, to our knowledge, there is no modelling work done for zinc-ion batteries. Within our contribution, we combine a description of complex formation with a dynamic cell model. The electrolyte speciation significantly influences the transport properties of the electrolyte as well as its stability. With our cell model, we predict the performance and rate-dependent behavior of commonly used materials. With this, we identify system-requirements and pitfalls in the ongoing optimization of aqueous zinc-ion batteries. This work is supported by the Federal Ministry of Education and Research (BMBF) via the project ZIB. Literature [1] S. Clark, N. Borchers, Z. Jusys, R. J. Behm, and B. Horstmann, Aqueous Zinc Batteries. 2020. [2] C. Xu, B. Li, H. Du, and F. Kang, “Energetic Zinc Ion Chemistry: The Rechargeable Zinc Ion Battery,” Angew. Chemie Int. Ed., vol. 51, no. 4, pp. 933–935, Jan. 2012, doi: 10.1002/anie.201106307. [3] B. Tang, L. Shan, S. Liang, and J. Zhou, “Issues and Opportunities Facing Aqueous Zinc-ion Batteries,” Energy Environ. Sci., pp. 3288–3304, 2019, doi: 10.1039/c9ee02526j. [4] J. Huang, Z. Guo, Y. Ma, D. Bin, Y. Wang, and Y. Xia, “Recent Progress of Rechargeable Batteries Using Mild Aqueous Electrolytes,” Small Methods, vol. 3, no. 1, p. 1800272, Jan. 2019, doi: 10.1002/smtd.201800272. [5] S. Clark et al., “Designing Aqueous Organic Electrolytes for Zinc-Air Batteries: Method, Simulation, and Validation,” Adv. Energy Mater., vol. 10, no. 10, p. 1903470, Mar. 2020, doi: 10.1002/aenm.201903470. Figure 1: Schematic of the interaction of the evaluation of electrolyte composition and the cell model. Illustration on the left adapted from [1] Figure 1
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