490296 Block-Copolymer Derived Nanoporous Carbon Membranes for High Throughput Gas Separation

Kumar Varoon Agrawal, Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland and Mostapha Dakhchoune, ISIC, EPFL, Sion, Switzerland

Ultrathin, gas-selective membranes are highly desired to reduce the total area for a given membrane operation, reducing capital and operating costs, as well as production time and complexity for a potential scale-up. Moreover, such membranes are expected to increase the overall energy-efficiency.

Nanoporous carbon films can be obtained by pyrolysis of block-copolymer thin films. However, for their application in high permeance membrane, a crack-free synthesis on a macroporous support is not trivial. Herein, a gas-selective nanoporous carbon (NPC) membrane is reported1 which displayed a gigantic hydrogen permeance (5.9 million GPU) that is several orders of magnitude higher than the membranes in the literature (barring the bilayer graphene membrane reported by Celebi et al.).2 A moderate H2/CO2 ideal selectivity of 4.3 was obtained.

A defect-free, ultra-high flux nanoporous carbon film was synthesized by optimizing the synthesis and transfer protocols. SEM and TEM images reveal the crack-free mesoporous structure with an average pore size of 20 ± 16 nm. Permeances of He and CH4 were tested at 25 °C and at 100 °C, whereas H2, N2 and CO2 were tested in the temperature range of 25-300 °C. NPC exhibited an extremely high permeance (above 1 million GPU) for all the gases. The gas permeance scaled inversely to square root of molecular weight in the temperature range of 25-250 °C, confirming Knudsen transport regime attributed to the mesoporous structure of the NPC film.

The NPC film was stable up to a transmembrane pressure of 4 bar. XPS data confirmed that NPC film primarily consisted of C-C bonded structure (284.8 eV), with only a small contribution of C-O bonds (286.7 eV), which typically arise from the C-O-C and C-OH groups on the surface of the film.

The ultrahigh hydrogen permeance (5.9 GPU), a moderate gas selectivity (H2/CO2 ideal selectivity of 4.3) and a high temperature stability (250 °C) make NPC film highly attractive in separation of gases.

References

1. Dakhchoune M. et. al, Patent Application, PCT/EP2017/057684

2. Celebi, K. et. al, Science. 344, 289-292 (2014)


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