Realizing small-flake graphene oxide membranes for ultrafast size-dependent organic solvent nanofiltration

Lina Nie; Kunli Goh; Yu Wang; Jaewoo Lee; Yinjuan Huang; H Enis Karahan; Kun Zhou; Michael D Guiver; Tae-Hyun Bae

doi:10.1126/sciadv.aaz9184

Realizing small-flake graphene oxide membranes for ultrafast size-dependent organic solvent nanofiltration

Sci Adv. 2020 Apr 24;6(17):eaaz9184. doi: 10.1126/sciadv.aaz9184. eCollection 2020 Apr.

Authors

Lina Nie¹, Kunli Goh^{1

2}, Yu Wang³, Jaewoo Lee², Yinjuan Huang⁴, H Enis Karahan^{1

2}, Kun Zhou³, Michael D Guiver^{5

6}, Tae-Hyun Bae^{1

7}

Affiliations

¹ School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore 637459, Singapore.
² Singapore Membrane Technology Centre, Nanyang Environment and Water Research Institute, Nanyang Technological University, Singapore 637141, Singapore.
³ Environmental Process Modelling Centre, Nanyang Environment and Water Research Institute, Nanyang Technological University, Singapore 637141, Singapore.
⁴ School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore.
⁵ State Key Laboratory of Engines, School of Mechanical Engineering, Tianjin University, Tianjin 300072, China.
⁶ Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China.
⁷ Department of Chemical and Biomedical Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-338, Republic of Korea.

Abstract

Membranes for organic solvent nanofiltration (OSN) or solvent-resistant nanofiltration (SRNF) offer unprecedented opportunities for highly efficient and cost-competitive solvent recovery in the pharmaceutical industry. Here, we describe small-flake graphene oxide (SFGO) membranes for high-performance OSN applications. Our strategy exploits lateral dimension control to engineer shorter and less tortuous transport pathways for solvent molecules. By using La³⁺ as a cross-linker and spacer for intercalation, the SFGO membrane selective layer was stabilized, and size-dependent ultrafast selective molecular transport was achieved. The methanol permeance was up to 2.9-fold higher than its large-flake GO (LFGO) counterpart, with high selectivity toward three organic dyes. More importantly, the SFGO-La³⁺ membrane demonstrated robust stability for at least 24 hours under hydrodynamic stresses that are representative of realistic OSN operating conditions. These desirable attributes stem from the La³⁺ cross-linking, which forms uniquely strong coordination bonds with oxygen-containing functional groups of SFGO. Other cations were found to be ineffective.

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