Bottom-up synthesis of graphene films hosting atom-thick molecular-sieving apertures

Luis francisco Villalobos, Cédric Van goethem, Kuang-Jung Hsu, Shaoxian Li, Mina Moradi, Kangning Zhao, Mostapha Dakhchoune, Shiqi Huang, Yueqing Shen, Emad Oveisi, Victor Boureau, Kumar varoon Agrawal

Research output: Contribution to journalArticlepeer-review

14 Citations (SciVal)

Abstract

Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misoriented grains generates molecular-sized pores in the lattice. The density of pores is comparable to that obtained by the state-of-the-art postsynthetic etching (1012 cm−2) and is up to two orders of magnitude higher than that of molecular-sieving intrinsic vacancy defects in single-layer graphene (SLG) prepared by chemical vapor deposition. The porous nanocrystalline graphene (PNG) films are synthesized by precipitation of C dissolved in the Ni matrix where the C concentration is regulated by controlled pyrolysis of precursors (polymers and/or sugar). The PNG film is made of few-layered graphene except near the grain edge where the grains taper down to a single layer and eventually terminate into vacancy defects at a node where three or more grains meet. This unique nanostructure is highly attractive for the membranes because the layered domains improve the mechanical robustness of the film while the atom-thick molecular-sized apertures allow the realization of large gas transport. The combination of gas permeance and gas pair selectivity is comparable to that from the nanoporous SLG membranes prepared by state-of-the-art postsynthetic lattice etching. Overall, the method reported here improves the scale-up potential of graphene membranes by cutting down the processing steps.
Original languageEnglish
JournalProceedings of the National Academy of Sciences
Volume118
Issue number37
Early online date7 Sept 2021
DOIs
Publication statusPublished - 14 Sept 2021
Externally publishedYes

Bibliographical note

We acknowledge the host institution École Polytechnique Fédérale de Lausanne (EPFL) for generous support. We gratefully acknowledge Shell for financial support. Parts of the project were funded by the Swiss National Science Foundation, Assistant Professor Energy Grant (PYAPP2_173645), and European Research Council Starting Grant (805437-UltimateMembranes). K.-J.H. acknowledges the Taiwan-EPFL PhD Scholarship program funded by the Ministry of Education, Taiwan. C.V.G. is grateful to Research Foundation Flanders (FWO) for a junior postdoctoral fellowship (12ZQ420N). We thank Aurelien Bornet for his assistance in the NMR analysis.

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