Super‐Assembled Multi‐Level Asymmetric Mesochannels for Coupled Accelerated Dual‐Ion Selective Transport

Asymmetric nanofluidic devices hold great potential in energy conversion applications. However, most of the existing asymmetric nanofluidic devices remain a single-level asymmetric structure and a single-ion selective layer, which results in weak ion selectivity and limited energy conversion efficiency. Herein, a multi-level asymmetric mesoporous carbon/anodized aluminum/mesoporous silica (MC/AAO/MS) nanofluidic device with abundant and ordered mesochannels is constructed from super-assembly strategy. The resultant MC/AAO/MS exhibits diode-like ion transport and outstanding ion storage-release performance. Importantly, MC/AAO/MS couples the MC and MS dual-ion selective layers, which ensures a high ionic conductance and evidently enhances the cation selectivity. Thereby, the MC/AAO/MS demonstrates ascendant salinity gradient energy conversion performance. The power density and conversion efficiency can reach up to 5.37 W m-2 and 32.79%, respectively. Noteworthy, a good energy conversion performance of 63 mW m-2 can still be achieved upon high working area, outperforming 300% of the performance of MC/AAO and MS/AAO single-level asymmetric nanochannels. Theoretical calculation further verifies that the multi-level asymmetric structure and dual-ion selective transport are the reason for the enhanced cation selectivity and energy conversion efficiency. This work opens a new avenue for constructing multi-level asymmetric structured nanofluidic devices for various applications.