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Atomically thin molecular carbon nanomembranes (CNMs) with intrinsicsub-nanometer porosity are considered as promising candidates for nextgeneration filtration and gas separation applications due to their extremelylow thickness, energy efficiency and selectivity. CNMs are intrinsically porouswhich is advantageous over other 2D materials such as graphene and transitionmetal dichalcogenides where defects and pores need to be introduced aftersynthesis. It was already discovered that water and helium permeate through4,4-terphenylthiol (TPT) CNM above the limit of detection. Additionally, thepermeation of water vapour was nonlinear against its pressure and 1000 strongerthan permeation of helium despite their similar kinetic diameters. However,there was no clear permeation mechanism which could explain permeation of bothspecies. Here, we demonstrate that permeation of all gas species is defined bytheir adsorption. We performed gas permeation measurements through TPT CNM atdifferent temperatures and found that all measured gases experienced anactivation energy barrier which correlated with their kinetic diameters.Furthermore, we identified that entropy loss during adsorption and permeationis the fundamental reason of strong nonlinear permeation of water. Our resultsalso demonstrated that adsorption plays a major role in permeation of allgases, not just water.

Gas transport mechanisms through molecularly thin membranes