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96 Natl Sci Rev, 2017, Vol. 4, No. 1 REVIEW (a) 1.5 1.4 1.3 1.2 1.1 1.0 0.9 0.8 (b) Cycle No. 10 11 12 13 14 15 16 17 18 19 3.0 3.5 4.0 4.5 5.0 5.5 6.0 Time / h (c) 3.0 2.7 2.4 2.1 1.8 1.5 1.5 M 0 10 20 30 40 50 60 Specific capacity / Ah L-1 (d) 3.0 2.5 2.0 1.5 1.0 0.5 0.0 1.6 1.4 1.2 1.0 0.8 0.6 012345 Time / h Cell volatage Anode-reference voltage 165 mAh/g 121 mAh/g 168 mAh/g 134 mAh/g 0 5 10 15 20 25 30 Time / h Figure 4. (a) Typical charge/discharge curves for ZIB systems at 1.5 M ZnI2 [37] (Copyright 2015 NPG). (b) Representative voltage versus time curves during 100 charge–discharge cycles at 100 mA/cm2, recorded between the 10th and 19th cycles [56] (Copyright 2015 AAAS). (c) Typical cycling voltage curves of the flow cell using 0.5 M FL/0.5 M DMBBM/1.0 M TEA– TFSI/MeCN at 15 mA/cm2 [76] (Copyright 2015 Wiley). (d) Two iterations of injection and galvanostatic cycling for a full lithium-ion flow cell operating between 0.5 and 2.6 V at C/8 rate. Suspensions are 20 vol% LiCoO2, 1.5 vol% Ketjen black and 10 vol% Li4Ti5O12, 2 vol% Ketjen black, both in 1 M LiPF6 in dimethyl carbonate [87] (Copyright 2011 Wiley). aqueous solutions as the catholytes on the other side. To prevent the reaction of Li metal and water, a dense solid electrolyte separator (e.g. LISICON: Li1+x+3z Alx (Ti,Ge)2−x Si3z P3−z O12 ) with high Li-ion conductivity is a critical component of this configuration. Investigations of Li systems have led to high interest in the use of sulfur, which is widely available and very inexpensive compared to other materials. The high solubility of polysulfide species also could also lead to battery systems that possess high energy densities (Table 1). Figure 3d shows ternary phase diagrams of Lix Sy . The theoretical sulfur capacity can be as high as 1672 mAh/g. Cui’s group [42] and Liu’s group [43] studied rechargeable redox-flow Li- S cells using traditional non-aqueous electrolytes. However, a critical problem in the liquid cell is precipitation of short-chain lithium sulfides. An interesting approach was developed by Zhou et al. [44] and Visco et al. [45,46]. Both groups proposed aqueous lithium–polysulfide batter- ies, which are based on a short-chain lithium sulfides (Li2 S4 –Li2 S) redox reaction. In this sys- tem, a Li-ion conductive glass separator (LATP: Li1.35 Ti1.75 Al0.25 P2.7 Si0.3 O12 ) isolates the Li metal and aqueous polysulfide electrolytes. The battery shows an OCV of approximately 2.67 V. The unique advantages of aqueous lithium–polysulfide batteries are that the Li2 S4 –Li2 S redox couple possesses high solubility (over 5.0 M [46,47] in the aqueous electrolyte, leading to a high energy density of 387 Wh/L. The LATP separator impedes the polysulfide shuttle during cycling and prevents lithium dendrite growth. However, the reduction of TiIV in the separators (i.e. LATP or LISICON) at low potential (<1.6 V vs. Li+/Li) makes it unstable when in direct contact with metallic Li. Therefore, a buffer layer is required to separate the glass ceramic from Li during long-term operation. Other inorganic materials, such as FeCl3 [41], K3Fe(CN)6 [48], LiI [49] and LiBr [50], can reach a high concentration in water and were also stud- ied for use as the cathode materials. The correspond- ing cells all demonstrated good cycling performance (except for FeCl3, which has a low pH), high cell voltage (>2.5 V) and high energy density. However, the low conductivity of the solid electrolyte separa- tor (∼10–4 S/cm vs. 0.1 S/cm for Nafion) produced a smaller operating current density and, therefore, a lower power output. Organic flow battery Although inorganic redox materials have attracted widespread attention, organic redox materials can offer more flexibility to tune the redox activity, sol- ubility and stability. In 2014, the Aziz group [51] and Narayanan group [52] proposed the use of a water-soluble, metal-free organic redox couple (i.e. quinone-based) in RFBs. Quinone derivatives are attractive because of their low cost ($5–$10/kg vs. $27/kg for vanadium) and their availability from bi- ological processes. Voltage / V Voltage / V Cell voltage / V Cell volaage / V Downloaded from https://academic.oup.com/nsr/article/4/1/91/2866462 by guest on 11 January 2023PDF Image | Progress in low cost redox flow batteries energy storage
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