Role of Oxygen Functionalities in Graphene Oxide Architectural Laminate Subnanometer Spacing and Water Transport

TL;DR

This study explores how oxygen functionalities in graphene oxide influence its layered structure and water transport properties, providing insights for designing more effective GO membranes for separation applications.

Contribution

It introduces a controlled synthesis method for GO laminates and correlates chemical modifications with water permeability, advancing understanding of nanoscale water transport mechanisms.

Findings

GO nanochannel height controls water permeability

Basal oxygen functionalities induce a no-slip Darcy-like flow regime

Chemical and morphological characterization accelerates membrane design

Abstract

Active research in nanotechnology contemplates the use of nanomaterials for engineering applications. However, a primary challenge is understanding the effects of nanomaterial properties on industrial device performance and translating unique nanoscale properties to the macroscale. One emerging example is graphene oxide (GO) membranes for separation processes. Thus, here we investigate how individual GO properties can impact layered GO characteristics and water permeability. GO chemistry and morphology were controlled with easy-to-implement photo-reduction and sonication techniques and were quantitatively correlated offering a valuable tool to speed up the characterization process. For example, one could perform chemical analysis and concurrently obtain morphology information or vice versa. Chemical GO modification allows for fine control of GO oxidation state and GO laminate nanoarchitecture enabling controlled synthesis of a GO architectural laminate (GOAL). The GOAL can be considered as the selective layer of the membrane created by interconnected sub-nanometer channels, characterized by a length and a height (i.e., GO spacing), through which water molecules permeate. Water permeability was measured for eight GOAL characterized by different GO chemistry and morphology, and indicate that GO nanochannel height dictates water transport. The simulations indicate a no-slip Darcy-like water transport regime inside the GOAL due to the presence of basal oxygen functionalities. The experimental and simulation evidence presented in this letter help create a clearer picture of water transport in GO and can be used to rationally design more effective and efficient GO membranes.