Electrochemical treatment of saline or brackish water by capacitive deionization (CDI) is a novel resource-saving solution to ensure the availability of freshwater resources in the environment. MOF (metal–organic framework) derived carbon as a novel carbonaceous material in CDI has received considerable research attention. Among them, ZIF-L-derived carbon (ZC) suffers from problems such as self-aggregation, poor mesoporous structure, and low electrical conductivity, which lead to poor CDI performance. In this paper, a strategy of ZIF-L coated with polydopamine (PDA) is proposed to solve the above problems. When the amount of PDA was 0.5 g, ZIF-L@PDA0.5-derived carbon composite (ZPC0.5) is obtained for efficient capacitive deionization. The ZPC0.5 composite not only maintains the 2D leaf shaped structure consistent with ZIF-L, exposing more active sites, but also has an elevated mesopore occupancy ratio to promote solution diffusion. Meanwhile, the interaction between PDA and ZIF-L makes the ZPC0.5 have a cavity structure, which improves the mass transfer capacity. The resulting ZPC0.5 composite has a specific capacitance (165.8F g−1) that is 3.86 times higher than that of ZC (42.9F g−1). Consequently, in 1.2 V, 500 mg/L NaCl solution, the symmetric CDI cell ZPC0.5//ZPC0.5 exhibits an excellent desalination capacity (29.6 mg/g), which is 2.69 times that of the ZC//ZC.
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