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nm. Similarly, the shift in the 3T2g band indicates the presence of sulfate anions complexed 2- 1+ [V.SO4 .5(H2O)] cation in the electrolyte solution. abc Figure 4. Geometry-optimized structures for (a) pristine [Vn+6(H2O)]n+ (b) sulfate complexed [V(SO4)2-6(H2O)]+ and (c) chlorine complexed [VCl.6(H2O)] (n-1)+ using DFT theory with PBE functional and QZ4P basis electron set incorporated in ADF 2010 package. The vanadium, oxygen, chlorine, sulfate and proton atoms are represented as pink, red, green, yellow and white spheres, respectively. The 3T2g band shift caused by the sulfate complexation was confirmed by comparing with the electronic spectra of pure sulfate and pure chloride based V3+ solutions with the sulfuric acid and hydrochloric acid solvent, respectively. The 3T2g peak of the chloride-based system was observed at 578 nm, similar to the [V3+6(H2O)]3+ molecule in crystals, whereas the pure sulfuric acid solutions shows shifted peak at 610 nm (Figure 5(b)). This result further revealed the existence 2- 1+ of the sulfate complexed [V.SO4 .5(H2O)] species in the mixed acid electrolyte system. The study showed that the V3+ cation precipitation is mainly a solubility issue. Current electrolyte research is therefore focused on the stabilizing of the V3+ cation at the concentration higher than 2.5M. a Figure 5. The optical spectra of V3+ electrolyte solutions measured at room temperature (a) 0.5M, 1.0M, 1.5M, 2.0M and 2.5M V3+in mixed acid solution represented from bottom to top spectra, and (b) 1.5M V3+ in pure sulfate solution (bottom) mixed acid solution (middle) and pure chloride solution (top). The arrows represent the 3T1g → 3T2g and 3T1g → 3T1g transitions reported in literature for pristine [V3+6(H2O)]3+ cation. 9PDF Image | Redox Flow Batteries for Stationary Electrical Energy Storage
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