Tunable Surface Charge of Layered Double Hydroxide Membranes Enabling Osmotic Energy Harvesting from Anion Transport

Abstract Membrane‐based osmotic energy harvesting is a promising technology with zero carbon footprint. High‐performance ion‐selective membranes (ISMs) are the core components in such applications. Recent advancement in 2D nanomaterials opens new avenues for building highly efficient ISMs. However, the majority of the explored 2D nanomaterials have a negative surface charge, which selectively enhances cation transport, resulting in the underutilization of half of the available ions. In this study, ISMs based on layered double hydroxide (LDH) with tunable positive surface charge are studied. The membranes preferentially facilitate anion transport with high selectivity. Osmotic energy harvesting device based on these membranes reached a power density of 2.31 W m −2 under simulated river/sea water, about eight times versus that of a commercial membrane tested under the same conditions, and up to 7.05 W m −2 under elevated temperature and simulated brine/sea water, and long‐term stability with consistent performance over a 40‐day period. A prototype reverse electrodialysis energy harvesting device, comprising a pair of LDH membranes and commercial cation‐selective membranes, is able to simultaneously harvest energy from both cations and anions achieving a power density of 6.38 W m −2 in simulated river/sea water, demonstrating its potential as building blocks for future energy harvesting systems.