Facile Size-Selective Defect Sealing in Large-Area Atomically Thin Graphene Membranes for Sub-Nanometer Scale Separations

Cheng, Peifu; Kelly, Mattigan M.; Moehring, Nicole K.; Ko, Wonhee; Li, An-Ping; Idrobo Tapia, Juan Carlos; Boutilier, Michael H.; Kidambi, Piran R.

doi:10.1021/acs.nanolett.0c01934

Facile Size-Selective Defect Sealing in Large-Area Atomically Thin Graphene Membranes for Sub-Nanometer Scale Separations

Journal Article · Mon Jul 06 00:00:00 EDT 2020 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.0c01934· OSTI ID:1761634

Cheng, Peifu ^[1]; Kelly, Mattigan M. ^[1]; Moehring, Nicole K. ^[1]; ^[2]; ^[2]; Idrobo Tapia, Juan Carlos ^[2]; Boutilier, Michael H. ^[3]; ^[1]

Vanderbilt Univ., Nashville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Western Univ., London, ON (Canada)

Atomically thin graphene with a high-density of precise subnanometer pores represents the ideal membrane for ionic and molecular separations. However, a single large-nanopore can severely compromise membrane performance and differential etching between pre-existing defects/grain boundaries in graphene and pristine regions presents fundamental limitations. Here, we show for the first time that size-selective interfacial polymerization after high-density nanopore formation in graphene not only seals larger defects (>0.5 nm) and macroscopic tears but also successfully preserves the smaller subnanometer pores. Low-temperature growth followed by mild UV/ozone oxidation allows for facile and scalable formation of high-density (4–5.5 $$\times$$ 10¹² cm^–2) useful subnanometer pores in the graphene lattice. We demonstrate scalable synthesis of fully functional centimeter-scale nanoporous atomically thin membranes (NATMs) with water (~0.28 nm) permeance ~23$$\times$$ higher than commercially available membranes and excellent rejection to salt ions (~0.66 nm, >97% rejection) as well as small organic molecules (~0.7–1.5 nm, ~100% rejection) under forward osmosis. $$\times$$

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); ACS Petroleum Research Fund (ACS PRF); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1761634

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 8 Vol. 20; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
desalination
high density subnanometer pores
nanoporous atomically thin membranes (NATMs)
scalable graphene membranes
size-selective defect sealing
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Facile Size-Selective Defect Sealing in Large-Area Atomically Thin Graphene Membranes for Sub-Nanometer Scale Separations

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