Achieving rational and precise tuning of the structure and composition of electrode materials represents a promising strategy for enhancing the performance of capacitive deionization (CDI). However, this endeavor encounters significant challenges. Herein, we present an elaborately designed hierarchical porous MOF/LDH Hetero-Nanosheet array (NiCoMn-HNA) which could be used as anode for the efficient Cl− capture. The unique hierarchical and permeable configuration of NiCoMn-HNA offers extensive accessibility to active sites and facilitates rapid electrolyte diffusion, thereby establishing a convenient pathway for efficient charge and ion transfer. Consequently, this enhances both the overall efficiency and respective rates. Furthermore, the synergistic effect between NiCo-ZIF-L and NiCoMn-LDH hollow pseudocapacitive materials significantly contributes to the enhancement of both electrochemical performance and desalination capabilities in NiCoMn-HNA. Accordingly, the NiCoMn-HNA electrode demonstrated larger electrochemical capacitym outstanding salt adsorption capacity (103.1 mg g−1), and remarkable cyclic desalination stability (90.47 % retention rate). Density functional theory (DFT) calculations confirmed that the hollow structure of NiCoMn-HNA promotes efficient the interfacial charge transfer from NiCo-ZIF-L and NiCoMn-LDH, leading to enhanced ion transfer rate and decreased energy required for ion migration. This research introduces a novel strategy for the purposeful design of high-performance electrode materials to advance CDI technology.
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