Interlayer-Confined Redox Assembly Creates a Continuous, Addressable Phase for Coupled Mass-Energy Transport in Lamellar Membranes

Abstract Lamellar 2D membranes offer angstrom-to-nanometer transport pathways, but their interlayers are usually treated as passive channels rather than reactive nanospaces. Here we report an interlayer-confined redox assembly that converts graphene oxide (GO) galleries into a continuous, electronically addressable metal–carbon phase. Single-walled carbon nanotubes (SWCNTs) are incorporated as through-thickness conductive bridges that, together with defect-rich GO/SWCNT interfaces and interlayer confinement, facilitate the partial in situ reduction and nucleation of Ag+, generating an anchored interlayer network that preserves lamellar order while strengthening the membrane to 131 MPa. This phase also provides a functional readout of continuity through absorption-dominant electromagnetic attenuation (47 dB in the X band; SSE/t 9.14 × 104 dB cm2 g–1) and enables illumination-gated transport. The optimized membrane achieves an SFV/U of 74.17 in equimolar V/U feeds and 20.71 in spiked seawater, while maintaining 96.61–98.04% uranium rejection over 10 24-h cycles. Selectivity arises from dehydration-biased entry and interlayer uranium capture/reduction.