• Ar plasma treatment effectively enlarges the interlayer spacing of NiCoAl-LDHs, enhancing chloride ion diffusion and active site exposure.
• The flexible carbon cloth substrate improves electrical conductivity and prevents nanosheet agglomeration, enabling self-supporting electrodes without binders.
• The Ar-NiCoAl-LDHs@ACC electrode achieves a high salt removal capacity of 93.26 mg g−1 and a rapid rate of 0.27 mg g−1 s−1 at 1.2 V.
• The electrode exhibits excellent cycling stability with over 85% capacity retention after 100 cycles, demonstrating practical potential for brackish water desalination.
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