Performance and Lifetime of Intercalative Water Deionization Cells for Mono- and Divalent Ion Removal

Intercalative deionization (IDI) uses two cation intercalation electrodes separated by an anion exchange membrane in a symmetric cell design that has the potential to deliver electrochemically desalinated water in an energy- and water-efficient way. Here, we define and measure metrics to describe the performance and lifetime of IDI cells and compare them for NaCl and CaCl2 feed solutions. With 20 mM NaCl, NiHCF/AEM/NiHCF flow cells achieve 10 mM average concentration change at a productivity of 20 l/h/m2 and 5 mM average concentration change at 130 l/h/m2. In both cases the cells are operated at a 3C current rate and consume ~30 Wh/m3 of energy. With 10 mM CaCl2, the specific capacity and salt removal of IDI flow cells is ~4 times lower. NiHCF/NiHCF beaker cells with CaCl2 electrolyte suffer from strong capacity fade, while the same cells with NaCl electrolyte achieve 500 cycles without any capacity fade. Our post-mortem analysis using X-ray diffraction, secondary electron microscopy, energy dispersive X-ray spectroscopy, synchrotron-based X-ray absorption spectroscopy and micro X-ray fluorescence mapping reveals that NiHCF dissolves upon repeated intercalation with Ca2+, releasing residual K+, Ni2+ and Fe(CN)63, which precipitates as a crystalline decomposition product on the electrodes. This side reaction deprives the active material NiHCF of charge compensating Fe, and thus accounts for the observed capacity fade.