Capacitive deionization (CDI) is considered as a revolutionary desalination method to alleviate the global water crisis. However, the current carbon-based CDI cells are constrained by the inferior desalination efficiency, resulting from the undesirable pore structure and sluggish electron/ion transport. Herein, a new porogen of silicalite-1 is proposed for the tailorable fabrication of flexible porous carbon nanofibers (PCNFs) by electrospinning, carbonization and alkali etching, where the surface area, total pore volume, mechanical robustness, specific capacitance, and electrosorption performance of the developed PCNFs are associated with the silicalite-1 dosage. The symmetric CDI unit assembled by the freestanding PCNF membrane electrodes shows a state-of-the-art desalination capacity (38.64 mg g−1), a remarkable salt removal rate (12.1 mg g−1 min−1), a desirable charge efficiency (82.36 %), an acceptable energy consumption (0.668 Wh g−1), and a satisfactory cyclic durability, and such excellent deionization performance can be explained by that the abundant hierarchical pores, the large accessible surface area, and the interconnected conductive carbon network effectively expedite the electron/ion transport. Additionally, the home-made CDI device has a favorable desalination capability toward the high-ion concentration seawater from the Yellow Sea (Xiaomai Island). This work not only validates the feasibility of silicalite-1 as the pore-forming agent for the targeted preparation of flexible PCNFs, but also it highlights the potential of pore engineering in freestanding PCNFs for advanced CDI.

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