Enhanced Capacitive Deionization of Hollow Mesoporous Carbon Spheres/MOFs Derived Nanocomposites by Interface‐Coating and Space‐Encapsulating Design

Abstract Exploring new carbon‐based electrode materials is quite necessary for enhancing capacitive deionization (CDI). Here, hollow mesoporous carbon spheres (HMCSs)/metal‐organic frameworks (MOFs) derived carbon materials (NC(M)/HMCSs and NC(M)@HMCSs) are successfully prepared by interface‐coating and space‐encapsulating design, respectively. The obtained NC(M)/HMCSs and NC(M)@HMCSs possess a hierarchical hollow nanoarchitecture with abundant nitrogen doping, high specific surface area, and abundant meso‐/microporous pores. These merits are conducive to rapid ion diffusion and charge transfer during the adsorption process. Compared to NC(M)/HMCSs, NC(M)@HMCSs exhibit superior electrochemical performance due to their better utilization of the internal space of hollow carbon, forming an interconnected 3D framework. In addition, the introduction of Ni ions is more conducive to the synergistic effect between ZIF(M)‐derived carbon and N‐doped carbon shell compared with other ions (Mn, Co, Cu ions). The resultant Ni‐1‐800‐based CDI device exhibits excellent salt adsorption capacity (SAC, 37.82 mg g −1 ) and good recyclability. This will provide a new direction for the MOF nanoparticle‐driven assembly strategy and the application of hierarchical hollow carbon nanoarchitecture to CDI.