Holey Sheets Enhance the Packing and Osmotic Energy Harvesting of Graphene Oxide Membranes

Layered membranes assembled from two-dimensional (2D) building blocks such as graphene oxide (GO) are of significant interest in desalination and osmotic power generation because of their ability to selectively transport ions through interconnected 2D nanochannels between stacked layers. However, architectural defects in the final assembled membranes (e.g., wrinkles, voids, and folded layers), which are hard to avoid due to mechanical compliant issues of the sheets during the membrane assembly, disrupt the ionic channel pathways and degrade the stacking geometry of the sheets. This leads to degraded ionic transport performance and the overall structural integrity. In this study, we demonstrate that introducing in-plane nanopores on GO sheets is an effective way to suppress the formation of such architectural imperfections, leading to a more homogeneous membrane. Stacking of porous GO sheets becomes significantly more compact, as the presence of nanopores makes the sheets mechanically softer and more compliant. The resulting membranes exhibit ideal lamellar microstructures with well-aligned and uniform nanochannel pathways. The well-defined nanochannels afford excellent ionic conductivity with an effective transport pathway, resulting in fast, selective ion transport. When applied as a nanofluidic membrane in an osmotic power generation system, the holey GO membrane exhibits higher osmotic power density (13.15 W m^-2) and conversion efficiency (46.6%) than the pristine GO membrane under a KCl concentration gradient of 1000-fold.