Ion-Gated Gas Separation through Porous Graphene

Tian, Ziqi; Mahurin, Shannon M.; Dai, Sheng; Jiang, De-en

doi:10.1021/acs.nanolett.6b05121

Title: Ion-Gated Gas Separation through Porous Graphene

Journal Article · Thu Feb 23 00:00:00 EST 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.6b05121· OSTI ID:1348344

Tian, Ziqi ^[1]; Mahurin, Shannon M. ^[2];

^[3];

^[1]

Univ. of California, Riverside, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Porous graphene holds great promise as a one-atom-thin, high-permeance membrane for gas separation, but to precisely control the pore size down to 3–5 Å proves challenging. Here we propose an ion-gated graphene membrane comprising a monolayer of ionic liquid-coated porous graphene to dynamically modulate the pore size to achieve selective gas separation. This approach enables the otherwise nonselective large pores on the order of 1 nm in size to be selective for gases whose diameters range from 3 to 4 Å. We show from molecular dynamics simulations that CO₂, N₂, and CH₄ all can permeate through a 6 Å nanopore in graphene without any selectivity. But when a monolayer of [emim][BF₄] ionic liquid (IL) is deposited on the porous graphene, CO₂ has much higher permeance than the other two gases. We find that the anion dynamically modulates the pore size by hovering above the pore and provides affinity for CO₂, while the larger cation (which cannot go through the pore) holds the anion in place via electrostatic attraction. This composite membrane is especially promising for CO₂/CH₄ separation, yielding a CO₂/CH₄ selectivity of about 42 and CO₂ permeance of ~10⁵ GPU (gas permeation unit). We further demonstrate that selectivity and permeance can be tuned by the anion size, pore size, and IL thickness. The present work points toward a promising direction of using the atom-thin ionic liquid/porous graphene hybrid membrane for high-permeance, selective gas separation that allows a greater flexibility in substrate pore size control.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231

OSTI ID:: 1348344

Alternate ID(s):: OSTI ID: 1478376

Journal Information:: Nano Letters, Vol. 17, Issue 3; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 90 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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gas separation
ionic liquid

Title: Ion-Gated Gas Separation through Porous Graphene

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