While nanoporous graphene oxide (GO) is recognized as one of the most promising reverse osmosis desalination membranes, limited attention has been paid to controlling desalination performance through the large GO pores, primarily due to significant ion leakage resulting in the suboptimal performance of these pores. In this study, we employed a molecular dynamics simulation approach to demonstrate that Mg2+ ions, adhered to carboxylated GO nanopores, can function as gates, regulating the transport of ions (Na+ and Cl-) through the porous GO membrane. Specifically, the presence of divalent cations near a nanopore reduces the concentration of salt ions in the vicinity of the pore and prolongs their permeation time across the pore. This subsequently leads to a notable enhancement in salt rejection rates. Additionally, the ion rejection rate increases with more adsorbed Mg2+ ions. However, the presence of the adsorbed Mg2+ ions compromises water transport. Here, we also elucidate the impact of graphene oxidation degree on desalination. Furthermore, we design an optimal combination of adsorbed Mg2+ ion quantity and oxidation degree to achieve high water flux and salt rejection rates. This work provides valuable insights for developing new nanoporous graphene oxide membranes for controlled water desalination.

Pristine graphene oxide (GO)-based membranes have proven promising for molecular and ion separation owing to efficient molecular transport nanochannels, but their separation ability in an aqueous environment is limited by the natural swelling tendency of GO. To obtain a novel membrane with anti-swelling behavior and remarkable desalination capability, we used the Al2O3 tubular membrane with an average pore size of 20 nm as the substrate and fabricated several GO nanofiltration ceramic membranes with different interlayer structures and surface charges by fine-tuning the pH of the GO-EDA membrane-forming suspension (pH = 7, 9, 11). The resultant membranes could maintain desalination stability, whether immersed in water for 680 h or operated under a high-pressure environment. When the pH of the membrane-forming suspension was 11, the prepared GE-11 membrane showed a rejection of 91.5% (measured at 5 bar) towards 1 mM Na2SO4 after soaking in water for 680 h. An increase in the transmembrane pressure to 20 bar resulted in an increase in the rejection towards the 1 mM Na2SO4 solution to 96.3%, and an increase in the permeance to 3.7 L·m-2·h-1·bar-1. The proposed strategy in varying charge repulsion is beneficial to the future development of GO-derived nanofiltration ceramic membranes.

Graphene oxide (GO) is a promising two-dimensional building block for fabricating high-performance gas separation membranes. Whereas the tortuous transport pathway may increase the transport distance and lead to a low gas permeation rate, introducing spacers into GO laminates is an effective strategy to enlarge the interlayer channel for enhanced gas permeance. Herein, we propose to intercalate CO2 -philic MIL-101(Cr) metal-organic framework nanocrystals into the GO laminates to construct a 2D/3D hybrid structure for gas separation. The interlayer channels were partially opened up to accelerate gas permeation. Meanwhile, the intrinsic pores of MIL-101 provided additional transport pathways, and the affinity of MIL-101 to CO2 molecules resulted in higher H2 /CO2 diffusion selectivity, leading to a simultaneous enhancement in gas permeance and separation selectivity. The MIL-101(Cr)/GO membrane with optimal structures exhibited outstanding and stable mixed-gas separation performance with H2 permeance of 67.5 GPU and H2 /CO2 selectivity of 30.3 during the 120-h continuous test, demonstrating its potential in H2 purification application.

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.

Graphene oxide (GO) membranes with unique nanolayer structure have demonstrated excellent separation capability based on their size-selective effect, but there are few reports on achieving ion-ion separation, because it is difficult to inhibit the swelling effect of GO nano sheets as well as to precisely control the interlayer spacing d to a specific value between the sizes of different metal ions. Here, selective separation of uranium from acidic radioactive waste containing multication is achieved through a precise dual-adjustment strategy on d. It is found that GO swelling is greatly restricted in highly acidic solution due to protonation effect. Then the interlayer spacing is further precisely reduced to below the diameter of uranyl ion by increasing the oxidation degree of GO. Sieving uranyl ions from other nuclide ions is successfully realized in pH =3-3 mol L-1 nitric acid solutions.

Graphene oxide (GO) and its composite membranes have exhibited great potential for application in water purification and desalination. This article reports that a novel graphene oxide membrane (GOM) of ~5 µm thickness was fabricated onto a nylon membrane by vacuum filtration and cross-linked by amino acids (L-alanine, L-phenylalanine, and serine). The GOM cross-linked by amino acids (GOM-A) exhibits excellent stability, high water flux, and high rejection to metal ions. The rejection coefficients to alkali and alkaline earth metal ions through GOM-A were over 94% and 96%, respectively. The rejection coefficients decreased with an increasing H+ concentration. Metal ions (K+, Ca2+, and Fe3+) can be inserted into GOM-A layers, which enlarges the interlayer spacing of GOM-A and neutralizes the electronegativity of the membrane, resulting in the decease in the rejection coefficients to metal ions. Meanwhile, GOM-A showed quite high antibacterial efficiency against E. coli. With the excellent performance as described above, GOM-A could be used to purify and desalt water.

As increasing demand for hemodialysis (HD) treatment incurs significant financial burden to healthcare systems and ecological burden as well, novel therapeutic approaches as well as innovations and technological advances are being sought that could lead to the development of purification devices such as dialyzers with improved characteristics and wearable technology. Novel knowledge such as the development of more accurate kinetic models, the development of novel HD membranes with the use of nanotechnology, novel manufacturing processes, and the latest technology in the science of materials have enabled novel solutions already marketed or on the verge of becoming commercially available. This collaborative article reviews the latest advances in HD as they were presented by the authors in a recent symposium titled \"Frontiers in Haemodialysis,\" held on 12th December 2019 at the Royal Society of Medicine in London.

Developing a convenient and effective method to prepare single-atom catalysts at mild synthetic conditions remains a challenging task. Herein, a voltage-gauged electrofiltration method was demonstrated to synthesize single-atom site catalysts at room temperature. Under regulation of the graphene oxide membrane, a bulk Fe plate was directly converted into Fe single atoms, and the diffusion rate of Fe ions was greatly reduced, resulting in an ultralow concentration of Fe2+ around the working electrode, which successfully prevented the growing of nuclei and aggregating of metal atoms. Monatomic Fe atoms are homogeneously anchored on the as-prepared nitrogen-doped carbon. Owing to the fast photoelectron injection from photosensitizers to atomically dispersed Fe sites through the highly conductive supported N-C, the Fe-SAs/N-C exhibits an outstanding photocatalytic activity toward CO2 aqueous reduction into syngas with a tunable CO/H2 ratio under visible light irradiation. The gas evolution rates for CO and H2 are 4500 and 4950 μmol g-1 h-1, respectively, and the tunable CO/H2 ratio is from 0.3 to 8.8. This article presents an efficient strategy to develop the single-atom site catalysts and bridges the gap between heterogeneous and homogeneous catalysts toward photocatalytic CO2 aqueous reduction into syngas.

Stacked graphene oxide (GO) nano-sheets with plentiful nanopores incorporated onto polymeric membrane are promising for water purification. However, maintaining high water permeability without sacrificing separation efficiency remains a challenge. Delamination of the GO layer from the membrane surface is another bottleneck affecting the efficiency of the material. To solve those problems, we immobilized a chemically crosslinked GO composite layer with enlarged interlayer space on the surface of a novel catalytic membrane, which served as the support. The modified GO nanosheets-coated catalytic membranes showed excellent separation robustness with withstanding strong lateral shear force during 6 h filtration in a crossflow model. The as-prepared membrane showed high removal efficiencies to Congo red and Basic blue (99 % and 96 %, respectively) due to the surface-coated GO composite layer. Furthermore, while launching the catalytic function of the membrane with a trace amount of reducing agent (NaBH4), the GO-coated composite membrane successfully purified 50 ppm Methyl orange, 50 ppm Methylene blue, 50 ppm Rhodamine B and 0.272 mmol/L 4-Nitrophenol to break through the membrane rejection limitation of 500 Mw. Combining nano-filtration and catalysis, the GO-coated composite membranes showed great potential for the continuous purification of chemically contaminated water.

We show the experimental achievement of dry GO membranes with interlayer spacings in the range from 7.09 Å to 8.72 Å, tuned and fixed by salts. We found that the interlayer spacings were dominated by the anions or the groups with negative charges in between the GO membranes. Density functional theory (DFT) calculations reveal that the highly efficient tuning of the interlayer spacing in dry GO membranes is due to ion-π interactions on the graphene sheets, together with the steric effects of anions in between the GO sheets. The findings are helpful for extending their potential applications including chemical sensors, nanomaterial devices preparation, chemical catalysis and synthesis, and gas separation.