Molecular Self‐Assembly Enables Tuning of Nanopores in Atomically Thin Graphene Membranes for Highly Selective Transport
Name
Jang et al Manuscript_Revision1_Production.pdf
Description
Accepted version
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2.65 MB
Format
Adobe PDF
Checksum (MD5)
964c5f6276c87ba2206a1b377e9a661d
Author(s)
Jang, Doojoon
Bakli, Chirodeep
Chakraborty, Suman
Karnik, Rohit
Date Issued
February 3, 2022
Journal
Advanced Materials
Publisher
Wiley
Citation
D. Jang, C. Bakli, S. Chakraborty, R. Karnik, Molecular Self-Assembly Enables Tuning of Nanopores in Atomically Thin Graphene Membranes for Highly Selective Transport. Adv. Mater. 2022, 34, 2108940.
Version
Author's final manuscript
Abstract
Atomically thin membranes comprising nanopores in a 2D material promise to surpass the performance of polymeric membranes in several critical applications, including water purification, chemical and gas separations, and energy harvesting. However, fabrication of membranes with precise pore size distributions that provide exceptionally high selectivity and permeance in a scalable framework remains an outstanding challenge. Circumventing these constraints, here, a platform technology is developed that harnesses the ability of oppositely charged polyelectrolytes to self-assemble preferentially across larger, relatively leaky atomically thin nanopores by exploiting the lower steric hindrance of such larger pores to molecular interactions across the pores. By selectively tightening the pore size distribution in this manner, self-assembly of oppositely charged polyelectrolytes simultaneously introduced on opposite sides of nanoporous graphene membranes is demonstrated to discriminate between nanopores to seal non-selective transport channels, while minimally compromising smaller, water-selective pores, thereby remarkably attenuating solute leakage. This improved membrane selectivity enables desalination across centimeter-scale nanoporous graphene with 99.7% and >90% rejection of MgSO4 and NaCl, respectively, under forward osmosis. These findings provide a versatile strategy to augment the performance of nanoporous atomically thin membranes and present intriguing possibilities of controlling reactions across 2D materials via exclusive exploitation of pore size-dependent intermolecular interactions.
MIT Department
Massachusetts Institute of Technology. Department of Mechanical Engineering
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DOI of Published Version
https://doi.org/10.1002/adma.202108940
