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Batteries 2022, 8, 272 ered oxide cathode and lean electrolyte. Moreover, the 260 stable cycles were achieved without the extra stack pressure under room temperature. charge/discharge profiles in Figure 2d, the AFSMB cell based on the bi-salts electrolyte exhibits the lowest nucleation overpotential and the highest discharge capacity compared with traditional SIBs, SMBs, and amorphous carbon−coated current collector-based an- ode−free cells. Furthermore, a 200 Wh kg−1 AFSMB was successfully launched with a lay- as the cathode and the graphitic carbon–coated Al foil acting as the current collector with no Na as the cathode and the graphitic carbon−coated Al foil acting as the current collector with no Na contentattheanodeside.The0.9MNaPF and0.1MNaBF indiglymeisusedastheelectrolyte; content at the anode side. The 0.9 M NaPF6 6 and 0.1 M NaB4 F4 in diglyme is used as the electrolyte; (c) the calculated LUMO and HOMO values of the diglyme, NaPF and NaBF salts; (d) The initial (c) the calculated LUMO and HOMO values of the diglyme, Na6,PF6, and N4aBF4 salts; (d) The initial discharge/charge profiles of Na-ion battery, Na metal battery, amorphous and graphitic carbon– discharge/charge profiles of Na-ion battery, Na metal battery, amorphous and graphitic car- coated current collector based anode–free cells at a current rate of 0.5 C [23]. Reproduced with the bon−coated current collector based anode−free cells at a current rate of 0.5 C [23]. Reproduced with permission of ref. [23], copyright 2022 Springer Nature. the permission of ref. [23], copyright 2022 Springer Nature. Despite the excellent reversibility for sodium plating/stripping enabled by ether-based Despite the excellent reversibility for sodium plating/stripping enabled by ether- electrolytes, the majority of ether-based solvents are unable to support the high-voltage 5 of 20 Figure 2. Strategies for the optimization of electrolytes. (a) Comparison of the differences in the Figure 2. Strategies for the optimization of electrolytes. (a) Comparison of the differences in the solvation energies of Na++ with commonly used pure and mixture solvents; [12] copyright 2015 solvation energies of Na with commonly used pure and mixture solvents; [12] copyright 2015 American Chemical Society. (b) A representative AFSMB cell with the layered metal oxide serving American Chemical Society. (b) A representative AFSMB cell with the layered metal oxide serving based electrolytes, the majority of ether-based solvents are unable to support the high- charging process due to their inferior antioxidation properties [24]. To expand the potential volwtaingdeocwhaorfgienthgepr–rboacseesds deluecetrtolythtesi,r sitnrfaetreigoiresansuticohxaids aitnicorneapsrinogpethrteiecso[n2c4e]n.Ttroateioxnpaonf d the sodium salts [25], or using the zeolite molecular sieve film to regulate the solvation structure potential window of ether−based electrolytes, strategies such as increasing the concentra- have been proven to be viable [26]. The concentration electrolyte has been widely regarded tion of sodium salts [25], or using the zeolite molecular sieve film to regulate the solvation as an appropriate technique to solve the dendrite problem for Li/Na–metal batteries structure have been proven to be viable [26]. The concentration electrolyte has been due to their distinctive solvation structures [27,28]. To reduce the cost from the salts, widely regarded as an appropriate technique to solve the dendrite problem for researchers induced an “inert” diluent into the highly concentrated electrolyte (denoted as Li/Na−metal batteries due to their distinctive solvation structures [27,28]. To reduce the localized high-concentrated electrolyte), which maintains the original solvation structure cost from the salts, researchers induced an “inert” diluent into the highly concentrated of cation–anion aggregates [29]. Such a method also works for sodium–metal batteries. electrolyte (denoted as localized high-concentrated electrolyte), which maintains the orig- For instance, a localized high–concentrated electrolyte, i.e., 2.1 M NaFSI with DME and inablis(o2l,v2,a2t–itorniflustorruocetuhryel) oefthceart(iBoTnF−Ea)n(itohne magoglarer gratieosis[219:2]). cSouclhd eanambelethaodenadlsroitew-froereks for sodNiuampl−amtinegt/asltbriaptpteinrigesC.EFoasrhinigshtaansc9e9,%a lionctahleizNeda/hCiguhc−ecllo[n25c]e.nTtorafuterdthelrercetarcohlytthe,hi.ieg.h, 2.1 M reversibility of Na plating/stripping processes while expanding the oxidative stability, Lu NaFSI with DME and bis(2,2,2−trifluoroethyl) ether (BTFE) (the molar ratio is 1:2) could et al. rationally designed a beyond–concentrated electrolyte by a 3A zeolite molecular sieve film [26]. As shown in Figure 3a, a high-voltage AFSMB is built by coating a zeolite film on the Al current collector, where the free solvent in the pure diglyme-based electrolyte will bePDF Image | Anode-Free Rechargeable Sodium-Metal Batteries
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