Efficient Capacitive Deionization Using Natural Basswood-Derived, Freestanding, Hierarchically Porous Carbon Electrodes

Carbon electrodes are of great importance in constructing high-performance capacitive deionization (CDI) devices. However, the use of conventional carbon electrodes for CDI is limited because of their poor mechanical stability and low mass loading. Herein, we report a binder-free, freestanding, robust, and ultrathick carbon electrode derived from a wood carbon framework (WCF) for CDI applications. The WCF inherits the unique structure of natural basswood, containing straightly aligned channels interconnected with highly ordered, open, and hierarchical pores. A CDI device based on thick WCF electrodes (1200 μm, equal to a mass loading of 50 mg cm^-2) exhibits a remarkable areal salt adsorption capacity (SAC) of 0.3 mg cm^-2, a high volumetric SAC of 2.4 mg cm^-3, and a competitive gravimetric SAC of 5.7 mg g^-1. Also, the good mechanical strength and water tolerance of the WCF electrodes improve the cycling stability of the CDI device. Finite element simulations of ion transport behavior indicate that the unique structure of the WCF substantially facilitates ion transport within the ultrathick CDI electrodes. This work provides a viable route to the rational design of freestanding and ultrathick electrodes for CDI applications and offers insights into the structure-performance relationship of CDI electrodes.