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Figure 7. Alkali-Metal-Based RFBs Using Na or K Metal as Anodes (A) Simulated structures of liquid Na or Na-Cs alloy droplets on Na-BASE at 100C; the yellow balls represent Na atoms, and green ones represent Cs atoms. Reprinted with permission from Lu et al.69 Copyright 2014 Springer Nature. (B) Schematic of room-temperature Na-K alloy-based hybrid RFB with various catholyte selections. Reprinted from Baclig et al.71 Copyright 2018 Elsevier. (C) Charge and discharge profiles of Na2S8jBASEjNa-BP-DME batteries during cycling. Reprinted with permission from Yu and coworkers.72 Copyright 2017 Springer Nature. and coworkers reported a Na-based analog cell composed of a Na-metal anode, Na super ionic conductor (NASICON: Na3Zr2Si2PO12) solid electrolyte, and aqueous Na4Fe(CN)6 catholytes.67 NASICON-type electrolytes with the 3D crystalline struc- ture have been identified as a potential separator for Na-based RFBs because they could provide a high Na+ conductivity close to the Na-b00-Al2O3 (103 S cm1) and remain stable in the aqueous environment. On the other hand, to improve the interfacial contact with solid electrolyte or alleviate the safety con- cerns, the Na metal can be replaced by Na-Cs/Na-K liquid alloy or liquid Na- biphenyl species. Using the Na-Cs alloy anode in organic electrolytes, Shaw and co- workers reported a RFB containing a Na-BASE electrolyte.68 Nevertheless, the adopted vanadium aqueous catholyte (VOSO4/HCl/Na2SO4) was corrosive, toxic, and expensive, and the Na-BASE separator was not able to show long-term stability in the aqueous medium. Thus, Liu and coworkers took advantage of the good wetta- bility of Na-Cs liquid alloy on beta alumina ceramics at a relatively low temperature range (95$175C) to develop Na-S or Na-metal halide batteries that could be suc- cessfully operated at the intermediate temperature for a long cycle life (Figure 7A).69 By comparing the heights and widths of the droplets containing different ratios of Na versus Cs atoms, it is evident that higher Cs content will improve the wetting behavior of the Na-Cs liquid alloy on the membrane. On the basis of a similar strat- egy, they further reported a low-cost, high-energy-density, and long-cycle-life K-S battery with a K+-conducting alumina ceramic membrane.70 The Na-K alloy could also improve the wetting behavior, but it would damage the Na-b00-Al2O3. When us- ing the K-b00-Al2O3 as the separator, the same problem still existed for the Na metal. Fortunately, by simply replacing Na with K in both the ceramic membrane and anode, it would completely solve the possible ion exchange and poor wetting is- sues. Operated at the temperature of 150C, the designed battery exhibited an excellent cycle life with negligible capacity degradation over 1000 cycles. Further- more, Rugolo and coworkers found the Na-K liquid alloy could also have a good wet- ting with K-b00-alumina at room temperature.71 Acting as a robust K-ion-selective separator, the K-b00-alumina enabled the design of K-based RFBs when different aqueous or nonaqueous catholytes were employed (Figure 7B). Three representa- tive positive redox species (K3Fe(CN)6, Fc, and Br2) were selected to show the high working voltage over 3 V. Despite of the limited conductivity of K-b00-alumina, the prototype battery could still show a promising maximum power density of 65 mW cm2 at room temperature. Except for the liquid metal alloy, a new class Chem 5, 1964–1987, August 8, 2019 1977PDF Image | Development of Redox Flow Batteries Based on New Chemistries
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