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ACS Omega Article value is a remarkable result compared to that of previous research using a battery system (0.29 Wh/L).24 The maximum desalination capacity, which is an important parameter in capacitive-based electrochemical desalination technologies (calculated as the mass of deionized NaCl (mg) divided by the total mass of the electrodes (g)), was measured from an additional test at a voltage range of 0.05−0.85 V in a 0.5 M NaCl aqueous solution (see Figure S2 and Table S2). From one cycle of the desalination process, the average deionized NaCl concentration is 298 mM and the desalination capacity is approximately 59.9 mg/g. Note that the mass of salt removal in the system was the total amount of deionized NaCl during one cycle of the process (charging and discharging steps). This excellent desalination performance is explained by the fact that the system can deionize the source water during both the charging and discharging steps, as it overcomes a limitation of energy efficiency and capacity among electro- chemical desalination processes, which have a separate regeneration and create brine. Figure 3a,b shows the FESEM images of as-prepared NaNiHCF and NaFeHCF. To obtain ordered nanocube particles, we synthesized Prussian blue materials using kineti- cally controlled crystallization, which is a controllable crystal growth method that uses the addition of sodium citrate, as reported in previous research.38,39 In this method, sodium citrate served as a chelating agent that is coordinated with metal ions, and, then, the slowly released metal ions from the citrate complex are reacted with hexacyanoferrate ions. This slow nucleation and crystal growth allows for the formation of well- shaped nanocube particles, and the particle size can be controlled by adjusting the amount of citrate ions. From the SEM images, the morphology of the Prussian blue particles appears to be a well-crystallized nanocube structure that has a size distribution of 300−500 nm. Figure 3c shows the XRD patterns of the as-prepared NaNiHCF and NaFeHCF. The XRD pattern of NaNiHCF reveals that diffraction lines of NaNiHCF with indexes of 220, 420, 440, and 620 exhibit as a doublet by comparison with the structured Fe4[Fe(CN)6]3 (JCPDS 52-1970). Supported by the ICP-AES analysis results (the Na/(Ni + Fe) molar ratio of NaNiHCF and the Na/Fe molar ratio of NaFeHCF are 0.85/1 and 0.72/1, respectively), this distortion of the face-centered cubic (fcc) structure is interpreted by the presence of an excess amount of Na ions in the Prussian blue lattice, which indicates a rhombohedral structure.40−42 The XRD peaks of NaFeHCF have a strong line and are well indexed to an fcc structure (JCDPDS 73-0687), which indicates the high crystallinity of NaFeHCF particles. Figure 4 shows the electrochemical properties of the Prussian blue electrodes characterized by CV and galvanostatic charging/discharging in an electrochemical cell. The CV curves of the NaFeHCF and NaNiHCF electrodes in Figure 4a appear as broad redox peaks between −0.1 to 0.2 V (vs Ag/AgCl) and 0.4 to 0.6 V (vs Ag/AgCl); also, similar redox reaction properties are observed in both 1 M NaCl and seawater electrolytes. As expected from the difference of the redox reaction potential, the rechargeable battery system can be composed of NaNiHCF as a positive electrode and NaFeHCF as a negative electrode. Figure 4b,c shows the galvanostatic performance of the NaNiHCF/NaFeHCF full cell and the potential profiles of each electrode using a three-electrode system with a silver/silver chloride (KCl sat′) reference electrode in seawater. Closely related to the CV results, the Prussian blue electrodes exhibit a similar redox reaction 1657 Figure 3. SEM images of (a) NaNiHCF particles and (b) NaFeHCF particles. (c) The XRD patterns of NaNiHCF with reference to JCPDS no. 52-1907 (Fe4[Fe(CN)6]3) and NaFeHCF with reference to JCPDS no. 73-0687 (FeFe(CN)6) data. potential plateau at −0.1 to 0.3 V in the negative electrode and 0.4−0.8 V in the positive electrode. Figure 4d shows the galvanostatic cycling performance of the NaNiHCF/NaFeHCF full cell at a current density of 0.1 A/ gnegative between 0.10 and 0.80 V in a seawater solution. As shown in the results, the initial charge capacity was 56.2 mAh/ gnegative, which is higher than that of manganese oxide-based materials, such as Na0.44MnO2 and Na2Mn5O10 (35 mAh/g), that are used for capacitive-based desalination technologies. The retained capacity remains at 91.5% after 100 cycles, and the Coulombic efficiency stays above 92% (average: 92.9%), indicating its good stability even though the electrolyte was DOI: 10.1021/acsomega.6b00526 ACS Omega 2017, 2, 1653−1659PDF Image | Rocking Chair Desalination Battery Prussian Blue Electrodes
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