Journal
NANO LETTERS
Volume 20, Issue 8, Pages 5951-5959Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c01934
Keywords
nanoporous atomically thin membranes (NATMs); size-selective defect sealing; high density subnanometer pores; scalable graphene membranes; subnanometer separations; desalination
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Funding
- ACS PRF [59267-DNI10]
- NSF CAREER award [1944134]
- Vanderbilt University
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1944134] Funding Source: National Science Foundation
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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 x 10(12) 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 (similar to 0.28 nm) permeance similar to 23X higher than commercially available membranes and excellent rejection to salt ions (similar to 0.66 nm, >97% rejection) as well as small organic molecules (similar to 0.7-1.5 nm, similar to 100% rejection) under forward osmosis.
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