Tunable gating graphene oxide (GO) membranes with high water permeance and precise molecular separation remain highly desired in smart nanofiltration devices. Herein, bioinspired by the filtration function of the renal glomerulus, we report a smart and high-performance graphene oxide membrane constructed via introducing positively charged polyethylenimine-grafted GO (GO-PEI) to negatively charged GO nanosheets. It was found that the additional GO-PEI component changed the surface charge, improved the hydrophilicity, and enlarged the nanochannels. The glomerulus-inspired graphene oxide membrane (G-GOM) shows a water permeance up to 88.57 L m–2 h–1 bar–1, corresponding to a 4 times enhancement compared with that of a conventional GO membrane due to the enlarged confined nanochannels. Meanwhile, owing to the electrostatic interaction, it can selectively remove positively charged methylene blue at pH 12 and negatively charged methyl orange at pH 2, with a removal rate of over 96%. The high and cyclic water permeance and highly selective organic removal performance can be attributed to the synergic effect of controlled nanochannel size and tunable electrostatic interaction in responding to the environmental pH. This strategy provides insight into designing pH-responsive gating membranes with tunable selectivity, representing a great advancement in smart nanofiltration with a wide range of applications.

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Carbon nanomaterials have proven their wide applicability in molecular separation and water purification techniques. Here, an unzipped carbon nanotubes (CNT) embedded graphene oxide (GO) membrane (uCNTm) is reported. The multiwalled CNTs were longitudinally cut into multilayer graphene oxide nanoribbons by a modified Hummer method. To investigate the varying effects of different bandwidths of unzipped CNTs on their properties, four uCNTms were prepared by a vacuum-assisted filtration process. Unzipped-CNTs with different bandwidths were made by unzipping multiwalled CNTs with outer diameters of 0–10, 10–20, 20–30, and 30–50 nm and named uCNTm-1, uCNTm-2, uCNTm-3, and uCNTm-4, respectively. The uCNTms exhibited good stability in different pH solutions, and the water permeability of the composite membranes showed an increasing trend with the increase of the inserted uCNTm’s bandwidth up to 107 L·m–2·h–1·bar–1, which was more than 10 times greater than that of pure GO membranes. The composite membranes showed decent dye screening performance with the rejection rate of methylene blue and rhodamine B both greater than 99%.

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