Two-dimensional graphene oxide (GO) membranes are promising for molecular-scale separations. Laminar GO membranes usually involve liquid phase fabrications in aqueous solvents, whereas their assembly behaviors in organic solvents remain unexplored. Herein, we report a simple methodology for controlling assembly behaviors of laminar GO membranes in organic solvents by altering GO-solvent interactions. We experimentally and theoretically demonstrated that, governed by the competition between GO-solvent intermolecular interaction and GO intramolecular interaction, GO nanosheets displayed deverse disperse properties in different organic solvents, thereby determining their distinct assembly behaviors. Moreover, the membrane formation and structure and their relations to transport properties were studied through detailed investigations of laminar GO membranes assembled in selected organic solvents. The uniform and intact GO membranes built up by good solvents assistant assembly featured competitive organic solvent nanofiltration (OSN) performances. For example, the GO_DMSO membrane exhibited permeance of 66–76 L m⁻² h⁻¹ bar⁻¹ of methanol and rejection of more than 95% of dyes with molecular weights >600 g mol⁻¹, and the GO_DMF membrane achieved permeance of 26–32 L m⁻² h⁻¹ bar⁻¹ of methanol and rejection of more than 95% of dyes with molecular weights >400 g mol⁻¹. This work elucidates the property-structure-performance relationships of laminar GO membranes assembled in organic solvents, offering a straightforward paradigm for controllable assembly of laminar 2D-material membranes via facile solvents selection.

二维氧化石墨烯 (GO) 膜有望用于分子级分离。层流 GO 膜通常涉及在水性溶剂中的液相制造，而它们在有机溶剂中的组装行为仍未得到探索。在此，我们报告了一种通过改变 GO-溶剂相互作用来控制有机溶剂中层状 GO 膜组装行为的简单方法。我们通过实验和理论证明，在 GO-溶剂分子间相互作用和 GO 分子内相互作用之间的竞争控制下，GO 纳米片在不同的有机溶剂中表现出不同的分散特性，从而决定了它们不同的组装行为。而且，通过对在选定有机溶剂中组装的层状 GO 膜的详细研究，研究了膜的形成和结构及其与传输特性的关系。通过良好的溶剂辅助组件构建的均匀且完整的 GO 膜具有具有竞争力的有机溶剂纳滤 (OSN) 性能。例如，GO_DMSO膜表现出 66-76 L m ^-2  h ^-1 bar ^-1的甲醇渗透率和超过 95% 的分子量 >600 g mol ^-1的染料的截留率，GO _DMF膜实现了 26-32 的渗透率L m ^-2  h ^-1 bar ^-1甲醇和超过 95% 的分子量 >400 g mol ^-1的染料的排斥。这项工作阐明了在有机溶剂中组装的层状 GO 膜的性质-结构-性能关系，为通过简便的溶剂选择来可控组装层状 2D 材料膜提供了一个直接的范例。