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Sci Adv. 2019 Jan 25;5(1):eaav1851. doi: 10.1126/sciadv.aav1851. eCollection 2019 Jan.

Etching gas-sieving nanopores in single-layer graphene with an angstrom precision for high-performance gas mixture separation.

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Laboratory of Advanced Separations (LAS), École Polytechnique Fédérale de Lausanne (EPFL), Sion CH-1951, Switzerland.
State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials, College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China.


One of the bottlenecks in realizing the potential of atom-thick graphene membrane for gas sieving is the difficulty in incorporating nanopores in an otherwise impermeable graphene lattice, with an angstrom precision at a high-enough pore density. We realize this design by developing a synergistic, partially decoupled defect nucleation and pore expansion strategy using O2 plasma and O3 treatment. A high density (ca. 2.1 × 1012 cm-2) of H2-sieving pores was achieved while limiting the percentage of CH4-permeating pores to 13 to 22 parts per million. As a result, a record-high gas mixture separation performance was achieved (H2 permeance, 1340 to 6045 gas permeation units; H2/CH4 separation factor, 15.6 to 25.1; H2/C3H8 separation factor, 38.0 to 57.8). This highly scalable pore etching strategy will accelerate the development of single-layer graphene-based energy-efficient membranes.

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