(614e) Engineering Gas-Sieving Nanopores in Graphene with Sub-Å Resolution | AIChE

(614e) Engineering Gas-Sieving Nanopores in Graphene with Sub-Å Resolution


Huang, S. - Presenter, École Polytechnique Fédérale de Lausanne (EPFL)
Zhao, J., Nanjing Tech University
Agrawal, K. V., École Polytechnique Fédérale De Lausanne (EPFL)
Single-layer graphene-based membranes have been regarded as the ultimate gas separation membranes, capable of yielding ultrahigh gas permeance and an attractive molecular selectivity, attributing to their atomic thicknesses.1 However, despite their promise, the attractive performance of atom-thick graphene membranes in the size-selective separation of gas mixtures has not been realized. The development of these membranes face two major bottlenecks: 1) crack-free fabrication of large-area membranes; 2) develop a controllable lattice etching technique mitigating the trade-off between the pore density and the pore-size distribution (PSD).

Herein, we reported several novel approaches to achieve record-high gas separation performance from single-layer graphene-based membrane. A novel nanoporous-carbon-assisted graphene transfer technique was developed, enabling the transfer of relatively large area single-layer graphene onto a macroporous support without inducing cracks or tears.2 For the first time, gas-sieving from the intrinsic defects in the chemical vapor deposition derived graphene was observed. Attractive gas separation performances were achieved with the ultralow porosity of 0.025%. Furthermore, a synergistic strategy of decoupling pore-nucleation and pore-expansion on graphene lattice resulted in high-performance single-layer graphene membranes (H2 permeance of 1340 to 6045 gas permeation units (GPU); H2/CH4 separation factor of 15.6 to 25.1).3 Moreover, millisecond graphene gasification was developed to realize high pore-density and narrow PSD nanoporous single-layer graphene, yielding record gas separation performance CO2/N2 selectivity of 24.4 with corresponding CO2 permeance over 9550 gas permeation units.4 Overall, we demonstrate that graphene-based membranes are indeed capable of reaching the predicted high performance in gas separation.


(1) Wang, L.; Boutilier, M. S. H.; Kidambi, P. R.; Jang, D.; Hadjiconstantinou, N. G.; Karnik, R. Fundamental Transport Mechanisms, Fabrication and Potential Applications of Nanoporous Atomically Thin Membranes. Nature Nanotechnology 2017, 12, 509–522.

(2) Huang, S.; Dakhchoune, M.; Luo, W.; Oveisi, E.; He, G.; Rezaei, M.; Zhao, J.; Alexander, D. T. L.; Züttel, A.; Strano, M. S.; Agrawal, K. V. Single-Layer Graphene Membranes by Crack-Free Transfer for Gas Mixture Separation. Nature Communications 2018, 9, 1–11.

(3) Zhao, J.; He, G.; Huang, S.; Villalobos, L. F.; Dakhchoune, M.; Bassas, H.; Oveisi, E.; Agrawal, K. V. Etching Nanopores in Single-Layer Graphene with an Angstrom Precision for High-Performance Gas Separation. Science Advances 2019, 5, eaav1851.

(4) Huang, S.; Villalobos, L. F.; Li, S.; Babu, D. J., Vahdat, M. T., Oveisi E., Agrawal, K. V. High-permeance Single-Layer Graphene Membrane with A Molecular Sieving Resolution of 0.2 Å, Submitted.