Essence of the Enhanced Osmotic Energy Conversion in a Covalent Organic Framework Monolayer

Low membrane conductivity originated from a high membrane thickness has long been the "Achilles heel" of the conventional polymeric membrane, greatly hampering the improvement of the output power density in osmotic power generation. Herein, we demonstrate a molecularly-thin two-dimensional (2D) covalent organic framework (COF) monolayer membrane, featured with ultimate thickness, high pore density, and tight pore size distribution, which performs as a highly efficient osmotic power generator. Despite the large pore size up to 3.8 nm and relatively low surface charge density of 2.2 mC m-2, the monolayer COF membrane exhibits a high osmotic current density of 16.7 kA m-2 and an output power density of 102 W m-2 under 50 times the NaCl salinity gradient (0.5 M/0.01 M). This superior power density could be further improved to 170 W m-2 in the real seawater/river water gradient system. When the large pore size and low surface charge density are considered, this superior performance is not expected. Computational studies further reveal that the ultimate membrane permeability originated from the high membrane porosity, rather than ion selectivity, plays a dominant role in the production of high current density, especially under high salinity. This work provides an alternative strategy to realize improved output power density in ultrapermeable membranes.