Fei Yu, Xiaochen Zhang, Peng Liu, Bingbing Chen ¡ 5 authors
Abstract Metalâorganic frameworks (MOF) have attracted extensive attention due to their ultraâhigh specific surface area and tunable structure, the mechanism of direct utilization for capacitive deionization (CDI) defluorination remains undefined. Here, MILâ101(Cr) with ultraâhigh specific surface area, high water stability, and open metal sites (OMSs) is prepared by a hydrothermal method for defluorination of CDI. Carbon black is used as a âchainâ to connect Fâstored in the holes of MILâ101(Cr) (CrâMOF)as âblocksâ to enhance the conductivity and ion storage capacity of MILâ101(Cr)/carbon black electrodes (CrâMOF electrodes). This simple construction method avoids the process complexity of in situ synthesis and performs better. These easily constructed âblockchainâlikeâ CrâMOF electrodes exhibit excellent defluorination capacity (39.84 mg NaF g electrodes â1 ), low energy consumption (1.2 kWh kg NaF â1 ), and good stability. The coupling of the electrochemical redox reaction of Cr 3+ /Cr 4+ with confined water is investigated using in situ and ex situ analysis methods combined with density functional theory (DFT), resulting in an unprecedented defluorination mechanism for CrâMOF electrodes. This study opens up new ideas for the application of MOF in CDI, clarifies the removal mechanism of MOF, and lays a foundation for further promoting the application of raw materials with poor conductivity in the field of CDI.