A dynamic intercalation mechanism in pre-intercalation carbon nanosheets for capacitive deionization cells

Abstract

Given that carbon-based electrodes suffer from poor long-term stabilities and limited desalination capacity, the optimized charge storage mechanism used for improving desalination performance remains requisite. In this work, the KC-pre-intercalated carbon nanosheets (PCNs) with abundant conjugated carbonyl groups were designed via a one-step smelting method for the first time as a novel intercalation electrode in the symmetric capacitive deionization. Interestingly, below 500 mg/L, the physical electrical double-layer mechanism is mainly influential. Benefitting from the proposed dynamic intercalation mechanism, a remarkable ion removal capacity of 1.65 g g−1 and impressive cyclability of 300 cycles (97.96%) were observed in the high salt concentrations (>1000 mg/L) and simulated seawater system rather than pure NaCl solution. The ultrahigh adsorption capacity and prominent cycling stability make the PCNs-based device rank top three among these of all the symmetric CDI systems reported in the literatures so far. The Na+ ions are intercalated in the enlarged interlayer spacing without a host structure deformation, thus offering a high ion removal rate (2.04 mg g−1 min−1) and a low energy consumption (0.28 Wh g−1). Our work exemplifies the importance of engineering conjugated carbonyl groups and pre-intercalated structure to capacitive deionization for brine.