Ion Selectivity in Multilayered Stacked Nanoporous Graphene

Nanoporous graphene is an ideal candidate for molecular filtration as it can potentially combine high permeability with high selectivity at molecular levels. To make use of graphene in filtration setups, the defects formed during its growth and during the transfer of graphene to the carrier support pose a challenge. These uncontrolled pores can be avoided by stacking graphene layers, and then, controlled pores can be initiated with oxygen plasma. Here, we show that two-layer stacks provide the best balance of defect coverage and high selectivity compared with other stacks. Using the electrical characterization of ionic solutions in the standard diffusion cell, we compare the ionic transport and ionic selectivity of up to three-layered stacks of graphene that have been plasma-treated. We find that there is a decrease in the ionic selectivity of a two-layered stack as one more layer of graphene is added. We provide a model for this occurrence. Our results will be helpful for making practical and high-performance filtration systems from two-dimensional materials

Million-Fold Decrease in Polymer Moisture Permeability by a Graphene Monolayer

Flexible, transparent, and moisture-impermeable materials are critical for packaging applications in electronic, food, and pharmaceutical industries. Here, we report that a single graphene layer embedded in a flexible polymer reduces its water vapor transmission rate (WVTR) by up to a million-fold. Large-area, transparent, graphene-embedded polymers (GEPs) with a WVTR as low as 10^–6 g m^–2 day^–1 are demonstrated. Monolayered graphene, synthesized by chemical vapor deposition, has been transferred onto the polymer substrate directly by a very simple and scalable melt casting process to fabricate the GEPs. The performances of the encapsulated organic photovoltaic (OPV) devices do not vary even after subjecting the GEPs to cyclic bending for 1000 cycles. Accelerated aging studies of working OPV devices encapsulated in the GEPs show a 50% lifetime of equivalent to 1 000 000 min, which satisfies the requirements of organic electronics

Insights on Defect-Mediated Heterogeneous Nucleation of Graphene on Copper

The grain size of monolayer large area graphene is key to its performance. Microstructural design for the desired grain size requires a fundamental understanding of graphene nucleation and growth. The two levers that can be used to control these aspects are the defect density, whose population can be controlled by annealing, and the gas-phase supersaturation for activation of nucleation at the defect sites. We observe that defects on copper surface, namely dislocations, grain boundaries, triple points, and rolling marks, initiate nucleation of graphene. We show that among these defects dislocations are the most potent nucleation sites, as they get activated at lowest supersaturation. As an illustration, we tailor the defect density and supersaturation to change the domain size of graphene from <1 μm² to >100 μm². Growth data reported in the literature has been summarized on a supersaturation plot, and a regime for defect-dominated growth has been identified. In this growth regime, we demonstrate the spatial control over nucleation at intentionally introduced defects, paving the way for patterned growth of graphene. Our results provide a unified framework for understanding the role of defects in graphene nucleation and can be used as a guideline for controlled growth of graphene