4.8 Article

Mix-Then-On-Demand-Complex: In Situ Cascade Anionization and Complexation of Graphene Oxide for High-Performance Nanofiltration Membranes

Journal

ACS NANO
Volume 15, Issue 3, Pages 4440-4449

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c08308

Keywords

graphene oxide; ionic complexation; nanofiltration; poly(ionic liquid); confinement effect

Funding

  1. European Research Council (ERC) [NAPOLI-639720]
  2. Swedish Research Council [2018-05351]
  3. Verband der Chemischen Industrie e.V. (VCI) in Germany [Dozentenpreis 15126]
  4. Wallenberg Academy Fellow program in Sweden [KAW 2017.0166]
  5. Stockholm University Strategic Fund [SU FV-2.1.1-005]
  6. National Natural Science Foundation of China [21776003]

Ask authors/readers for more resources

The study introduced a new concept of mix-then-on-demand-complex for assembling 2D materials with polyelectrolytes, improving structural order and fabricating ultra-thin nanofiltration membranes with high water permeability and excellent dye rejection. Synergistic combination of hydrophobic confinement effect and supramolecular interactions in the membranes created interface transport nanochannels between GO and PIL that enhanced water transport efficiency.
Assembling two-dimensional (2D) materials by polyelectrolyte often suffers from inhomogeneous microstructures due to the conventional mixing-and-simultaneous-complexation procedure (mix-and-complex) in aqueous solution. Herein a mix-then-on-demand-complex concept via on-demand in situ cascade anionization and ionic complexation of 2D materials is raised that drastically improves structural order in 2D assemblies, as exemplified by classical graphene oxide (GO)-based ultrathin membranes. Specifically, in dimethyl sulfoxide, the carboxylic acid-functionalized GO sheets (COOH-GOs) were mixed evenly with a cationic poly(ionic liquid) (PIL) and upon filtration formed a well-ordered layered composite membrane with homogeneous distribution of PIL chains in it; next, whenever needed, it was alkali-treated to convert COOH-GO in situ into its anionized state COO--GO that immediately complexed ionically with the surrounding cationic PIL chains. This mix-then-on-demand-complex concept separates the ionic complexation of GO and polyelectrolytes from their mixing step. By synergistically combining the PIL-induced hydrophobic confinement effect and supramolecular interactions, the as-fabricated nanofiltration membranes carry interface transport nanochannels between GO and PIL, reaching a high water permeability of 96.38 L m(-2) h(-1) bar(-1) at a maintained excellent dye rejection 99.79% for 150 h, exceeding the state-of-the-art GO-based hybrid membranes. The molecular dynamics simulations support the experimental data, confirming the interface spacing between GO and PIL as the water transport channels.

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