Beyond Saline Electrolytes: Ultrafast and Selective Ion Transport in Gradient‐Ordered Hydrogel Electrolytes Enables High‐Rate and Ultra‐Stable Energy Storage

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ABSTRACT Aqueous ion batteries with traditional hydrogel electrolytes offer high safety, low cost, and simple manufacturing, but are hindered by slow ion transport, limiting fast charging applications. This study develops a gradient‐ordered hydrogel (GO‐hydrogel) electrolyte via centrifugal sieving. Through centrifugal shear and component design of sol, a gradient structure and a unilateral chain‐ordered layer are created. This unique structure enables high‐flux, high‐rate ion transport and ion selectivity, achieving a conductivity of 53.34 mS cm −1 . GO‐hydrogel enables aqueous energy systems to outperform liquid electrolytes in rate performance and conventional gels in cycling stability. Sodium‐ion batteries withstand 40 A g −1 and retain 92.69% capacity after 20 000 cycles at 5 A g −1 , while symmetric supercapacitors show no decay after 10 000 cycles at 1 A g −1 . This study is the first to construct gradient ordered ion transport channels via centrifugal shear force, providing a replicable strategy for gel material design in electrochemical energy storage, biomedicine, sensing, and other fields.

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