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D.-H. Nam, M.A. Lumley and K.-S. Choi Energy Storage Materials 37 (2021) 556–566 was examined galvanostatically at ± 4 mA cm−2 with cutoff potentials of 0.0 V and 0.9 V vs Ag/AgCl. The NiHCF electrode used as the work- ing electrode (geometric area of 1 cm2) contained ~11 mg of NiHCF. As the exact theoretical capacity of NiHCF cannot be accurately deter- mined because of the water content that varies with temperature and humidity, 60 mA g−1 was used as 1 C-rate in this study, which is a com- mon assumption made in the studies of PBA-based Na-storage electrodes [37]. Thus, ± 4 mA cm−2 is equivalent to ~ 6 C-rate. A BiOCl electrode (geometric area of 4 cm2) was used as the counter electrode. For all ex- periments, an Ag/AgCl (4 M KCl) reference electrode was placed near the working electrode to monitor the potential change of the working electrode during the cyclability tests. 4.6. Operation of Charging and Discharging Cells The operation of Charging Cell 1 composed of a NaTi2 (PO4 )3 elec- trode (geometric area of 4 cm2) and a Bi electrode (geometric area of 1 cm2) was galvanostatically tested in 0.6 M NaCl at 1.33 mA cm−2 (~0.5 C-rate based on the Bi electrode) until the capacity of the Bi elec- trode reached 100 mAh g−1. When the operation of Charging Cell 1 was complete, the Bi/BiOCl electrode was manually lifted from the so- lution, rinsed with DI water, and then moved to Charging Cell 2. In Charging Cell 2, the Bi/BiOCl electrode and a fully desodiated NiHCF electrode (geometric area of 4 cm2) were electrically connected and im- mersed in 70 mM HCl (pH 1.3). Then, Charging Cell 2 was galvanos- tatically operated at 1.33 mA cm−2 until the potential of the Bi/BiOCl electrode reached −0.4 V vs Ag/AgCl. When the operation of Charging Cell 2 was complete, the NiHCF electrode from Charging Cell 2 and the NaTi2(PO4)3 electrode from Charging Cell 1 were moved to Discharging Cell. These two electrodes were electrically connected and immersed in a 0.6 M NaCl solution. Discharging Cell was operated at a constant cur- rent of 1.33 mA cm−2 until the potential of the NiHCF electrode reached 0.15 V vs Ag/AgCl. In all experiments, the Ag/AgCl (4 M KCl) reference electrode was placed between the working electrode and the counter electrode to monitor changes in the individual potentials of both elec- trodes. 4.7. Determination of Na+ and Cl− removal efficiencies The actual concentrations of Na+ and Cl− present in the electrolyte of Charging Cell 1 were measured by a sodium ion meter (Horiba B- 722) and a chloride ion meter (Horiba 6560-10C) after passing a charge of 0, 9, 18, and 27 C. An undivided three-electrode cell consisting of a Bi electrode as the working electrode, a NaTi2 (PO4 )3 electrode as the counter electrode, and an Ag/AgCl electrode (4 M KCl) as the reference electrode was used for this experiment. A constant potential of 0.6 V vs. Ag/AgCl was applied to oxidize Bi to BiOCl. As the size of the Bi electrode in this experiment was limited, a 0.06 M NaCl solution was used to ensure that reliable changes in the Na+ and Cl− concentrations were measured by the sodium and chloride ion meters. For the chloride ion meter whose accuracy is considerably affected by the conductivity of the sample solution, 0.1 M KNO3 was added to the sample solution to provide optimum solution conductivity. The FE for ion removal was determined by dividing the measured ion concentration by the theo- retically expected ion concentration based on the charge passed. The resulting value was multiplied by 100% and is reported as a percentage. Declaration of competing interest There are no conflicts to declare. Acknowledgements This work was supported by the National Science Foundation (NSF) through grants CBET-1803496 and PFI-2016321 and the Draper Tech- nology Innovation Fund (University of Wisconsin-Madison). Supplementary materials Supplementary material associated with this article can be found, in the online version, at doi:10.1016/j.ensm.2021.02.037. References [1] P.A. Owusu, S. Asumadu-Sarkodie, A review of renewable energy sources, sustain- ability issues and climate change mitigation, Cogent. Eng. 3 (2016) 1167990. [2] B. Dunn, H. Kamath, J.–M Tarascon, Electrical energy storage for the grid: A battery of choices, Science 334 (2011) 928–935. [3] Z. Yang, J. Zhang, M.C.W. Kintner-Meyer, X. Lu, D. Choi, J.P. Lemmon, J. Liu, Elec- trochemical energy storage for green grid, Chem. Rev. 111 (2011) 3577–3613. [4] R.C. Armstrong, C. Wolfram, K.P. de Jong, R. Gross, N.S. Lewis, B. Boardman, A.J. Ragauskas, K. Ehrhardt-Martinez, G. Crabtree, M.V. Ramana, The frontiers of energy, Nat. Energy 1 (2016) 15020. [5] B. Zakeri, S. Syri, Electrical energy storage systems: A comparative life cycle cost analysis, Renew. Sustain. Energy Rev. 42 (2015) 569–596. [6] Y.Kim,G.–T.Kim,S.Jeong,X.Dou,C.Geng,Y.Kim,S.Passerini,Large-scalestation- ary energy storage: Seawater batteries with high rate and reversible performance, Energy Storage Mater. 16 (2019) 56–64. [7] J.B. Goodenough, K.-S. Park, The Li-ion rechargeable battery: A perspective, J. Am. Chem. Soc 135 (2013) 1167–1176. [8] D. Lin, Y. Liu, Y. Cui, Reviving the lithium metal anode for high-energy batteries, Nat. Nanotech. 12 (2017) 194–206. [9] M. Ko, S. Chae, J. Ma, N. Kim, H.-W. Lee, Y. Cui, J. Cho, Scalable synthesis of silicon– nanolayer-embedded graphite for high-energy lithium-ion batteries, Nat. Energy 1 (2016) 16113. [10] L. Lu, X. Han, J. Li, J. Hua, M. Ouyang, A review on the key issues for lithium-ion battery management in electric vehicles, J. Power Sources 226 (2013) 272–288. [11] H. Kim, J. Hong, K.–Y. Park, H. Kim, S.–W. Kim, K. Kang, Aqueous rechargeable Li and Na ion batteries, Chem. Rev. 114 (2014) 11788–11827. [12] D. Bin, F. Wang, A.G. Tamirat, L. Suo, Y. Wang, C. Wang, Y. Xia, Progress in aqueous rechargeable sodium-ion batteries, Adv. Energy Mater. 8 (2018) 1703008. [13] J.Shin,J.W.Choi,Opportunitiesandrealityofaqueousrechargeablebatteries,Adv. Energy Mater. 10 (2020) 2001386. [14] D. Kundu, E. Talaie, V. Duffort, L.F. Nazar, The emerging chemistry of sodium ion batteries for electrochemical energy storage, Angew. Chem., Int. Ed. 54 (2015) 3431–3448. [15] C. Vaalma, D. Buchholz, M. Weil, S. Passerini, A cost and resource analysis of sodi- um-ion batteries, Nat. Rev. Mater. 3 (2018) 18013. [16] M. Pasta, C.D. Wessells, Y. Cui, F.L. Mantia, A desalination battery, Nano Lett. 12 (2012) 839–843. [17] D.–H. Nam, K.–S. Choi, Bismuth as a new chloride-storage electrode enabling the construction of a practical high capacity desalination battery, J. Am. Chem. Soc. 139 (2017) 11055–11063. The Coulombic efficiency of the Bi electrode is ~104%, meaning that its dechlorination capacity is higher than its chlorination capacity. The capacities of Charging Cell 1 (100 mAh gBi−1) and Charging Cell 2 (105.29 mAh gBi−1) shown in Fig. S10a-b were determined based on the chlorination and dechlorination capacities of Bi, respectively. (The NaTi2 (PO4 )3 and NiHCF electrodes used in this study contained excess NaTi2 (PO4 )3 and NiHCF, respectively, and their total electrode capaci- ties were much greater than that of Bi.) Therefore, the sodiation capacity of NaTi2(PO4)3 during the operation of Charging Cell 1 was less than the desodiation capacity of NiHCF during the operation of Charging Cell 2. When sodiated NaTi2(PO4)3 and desodiated NiHCF were combined in Discharging Cell, the cell operation continued until NiHCF regained the same amount of Na+ that it had released in Charging Cell 2 (105.36 mAh gBi −1 ). Thus, the desodiation capacity of NaTi2 (PO4 )3 in Discharging Cell was greater than the sodiation capacity of NaTi (PO ) in Charg- 243 ing Cell 1. Because the initial NaTi2 (PO4 )3 electrode used in Charging Cell 1 was pre-sodiated and contained excess Na3Ti2(PO4)3, this discrep- ancy could be tolerated for a few cycles. However, when necessary, the NaTi2 (PO4 )3 electrode was additionally sodiated to maintain the Na+ content in the electrode as ~30% of its capacity. Another major effect of the capacity of Discharging Cell being greater than that of Charging Cell 1 is that it leads to an overestimated energy output and therefore an overestimated energy efficiency. (The energy output (input) is the product of the capacity and output (input) voltage.) Thus, in order to obtain a more accurate energy efficiency, which would have been obtained if the Coulombic efficiency of the Bi electrode was 100%, we normalized the capacities of all three cells to be identical (100 mAh). The results using normalized capacities are shown in Fig. 4. and results obtained using the as-obtained capacities are shown in Fig. S10. 565PDF Image | seawater battery with desalination capabilities
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