Moisture-Permeable, Humidity-Enhanced Gas Barrier Films Based on Organic/Inorganic Multilayers

Gas barrier films with water-vapor-permeability have exhibited broad application prospects in gas separation and dehumidification. Herein, multilayer films comprised of layered double hydroxides (LDH) nanosheets and carboxymethyl cellulose sodium (CMC) were fabricated via layer-by-layer assembly. The resulting (LDH/CMC) _n films show excellent gas barrier properties, which are ascribed to the significantly increased pathway for gas permeation originating from the large aspect ratio and high orientation of two-dimensional LDH nanosheets. Unlike traditional gas barrier films with nonselective blocking effect for various gases (including water vapor), the (LDH/CMC) _n films exhibit an unusual moisture permselective property. The moisture-permeable property was related to the hygroscopicity of CMC and hydrophilicity of LDH, which can enrich the water molecules from the surroundings and aggrandize the osmotic pressure for water vapor, resulting in an uncommon improvement of water vapor transmission. It is interesting to find that the (LDH/CMC) _n films exhibit enhanced gas (O₂, CO₂, CH₄, and N₂) barrier properties upon treatment in a humid environment, due to the formation of hydrogen bonds between the infiltrated water molecules and hydrophilic groups in CMC, thus padding the interstitial space of the CMC molecular chains and increasing the gas transmission path. The reduction of free volume and extension of the gas transmission path further enhance the gas barrier properties of (LDH/CMC) _n films. Moreover, the (LDH/CMC) _n films represent the water vapor permselective property in mixed gas (including O₂, CO₂, CH₄, N₂, and water vapor), while maintaining the barrier for other gases, which can be potentially applied in air dehydration and dehumidification of natural gas.