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Xiao et al. Energy Mater 2023;3:300007  https://dx.doi.org/10.20517/energymater.2022.84  Page 9 of 13


























                Figure 6. (A) Schematic illustration of ordered arrays on nickel foam as self-supported for flexible Zn-air battery [96]  Reproduced with
                permission  from  Ref. [96] . Copyright  2019  John  Wiley  &  Sons,  Inc.;  (B)  Schematic  presentation  of  nanocellulose  membrane
                functionalization and demonstration of flexible Zn-air  battery [98] . Reproduced with permission from  Ref. [98] . Copyright 2015 Royal
                Society of Chemistry.


               cycling stability, maintaining a capacity retention rate of 92% after 5000 cycles at a current density of 5C .
                                                                                                      [100]
               This work opens a direction for the development of long-lived flexible Zn-MnO .
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               PERSPECTIVES
               This review describes the overall landscape of aqueous Zn-based batteries, including Zn-ion batteries, Zn-
               air batteries, redox flow batteries, and flexible batteries. Within each classification, the basic working
               principle and recent research progress are summarized. Currently, there are still many obstacles that need to
               be removed on the road to the commercialization of Zn-based batteries. Therefore, two main perspectives
               related to battery material design and intrinsic mechanism exploration are given as follows:


               (1) Material design and optimization to improve electrochemical performance is still a challenge for various
               types of Zn-based battery configurations. For Zn-ion batteries, the search for materials that can withstand
               sustained multi-electron transfer while maintaining structural stability is strongly needed for both the
               intercalation and conversion cathodes. Electrocatalysts, with sufficient active sites, high activity and
               sufficient durability, are required in Zn-air batteries. The development of highly active cathode materials
               and cost-effective, stable and ion-conducting membranes is crucial for redox flow batteries. For flexible
               batteries, the mechanical flexibility and structural stability of battery materials are prerequisites for flexible
               devices, while the hydroxyl conductivity, water-holding ability, and alkali tolerance of gel electrolytes
               determine the performance of Zn-air batteries.

               (2) Apart from material design, the electrochemical behavior of electrode materials is still not well
               understood. Deeper mechanistic studies are desperately needed to further improve the electrochemical
               performance of Zn-based batteries. Taking Zn-air batteries as an example, although metal-based materials
               are widely used as bifunctional catalysts in Zn-air batteries, it was only recently revealed that their derived
               metal  hydroxides  are  the  real  active  sites  for  OER.  A  metal  hydroxide  layer  was  found  on  the
               Ba Sr Co Fe O -δ surface during the OER reaction. This phenomenon was also found when spinel
                        0.8
                            0.2
                              3
                 0.5
                    0.5
               CoFe Al O  was used as a catalyst. Therefore, further mechanistic understanding through in situ probing
                    0.25
                       1.75
                           4
               methods is strongly demanded to aid the search for better catalyst materials.
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