Enhanced Pseudo-Capacitance Process in Nanoarchitectural Layered Double Hydroxide Nanoarrays Hollow Nanocages for Improved Capacitive Deionization Performance

Layered double hydroxides (LDHs) are perceived as a hopeful capacitive deionization (CDI) faradic electrode for Cl^- insertion due to its tunable composition, excellent anion exchange capacity, and fast redox activity. Nevertheless, the self-stacking and inferior electrical conductivity of the two-dimensional structure of LDH lead to unsatisfactory CDI performance. Herein, the three-dimensional (3D) hollow nanocage structure of CoNi-layered double hydroxide/carbon composites is well designed as a CDI anode by cation etching of the pre-carbonized ZIF-67 template. C/CoNi-LDH has a unique 3D hollow nanocage structure and abundant pore features, which can effectively suppress the self-stacking of LDH sheets and facilitate the transport of ions. Moreover, the introduced amorphous carbon layer can act as a conductive network. When employed as the CDI anode, C/CoNi-LDH exhibited a high Cl^- removal capacity of 60.88 mg g^-1 and a fast Cl^- removal rate of 18.09 mg g^-1 min^-1 at 1.4 V in 1000 mg L^-1 NaCl solution. The mechanism of the Cl^- intercalation pseudo-capacitance reaction of C/CoNi-LDH is revealed by electrochemical kinetic analysis and ex situ characterization. This study provides vital guidance for the design of high-performance electrodes for CDI.