Environmental Remediation of Arsenate-Contaminated Groundwater Using a Graphene Oxide-Supported Cu-NPs/UiO-66(Zr)-NH₂...

Arsenic contamination, mainly in the arsenate (As(V)) form, continues to pose a serious threat to groundwater quality worldwide due to its long-term stability and toxicity at very low levels. Herein, we demonstrate, for the first time, a three-dimensional graphene oxide-based nanocomposite composed of Cu nanoparticle-doped, amino-functionalized UiO-66 (Cu/UiO-66-NH₂) anchored on a graphene oxide framework (Cu/UiO-66-NH₂@GO) as a novel and efficient nanosorbent for the rapid removal of As(V) in groundwater-like solutions. The nanocomposite was characterized by SEM and HRTEM to confirm the hybrid structure and by XRD, N₂ adsorption-desorption isotherms, and XPS to investigate crystallinity, porosity, and surface chemistry. The derived material exhibited a highly dispersed morphology and performed rapid arsenate solid-phase extraction to attain equilibration within 10 min and was effective for a wide pH range of 2-11. The best fit for the kinetic profiles was provided by the pseudo-second-order model. Interestingly, the maximum adsorption capacity of 747.9 mg g^-1 at pH 6.8 was achieved, demonstrating the benefits of the complementary pairing of dispersive GO sheets and Zr-MOF adsorption domains with Cu-derived active sites. Mechanistically, the enhanced uptake is ascribed to a combination of effects, including electrostatic pre-concentration, ligand exchange, and inner-sphere complexation at metal-oxo nodes; spectroscopic analysis (XPS and FTIR) suggests that the majority of arsenate is immobilized via a strong Zr-O-As bond at coordinatively unsaturated Zr centers, which is in line with t-ZrO₂-like surface domains formed within the nanocomposite. The embedded GO support inhibits further framework interpenetration and enhances active site availability and mass transport, leading to fast and high-capacity arsenate capture in groundwater samples with related conditions. Taken together, this work presents a powerful design concept that integrates unique GO-supported, Cu-modified UiO-66-NH₂ with Zr-O binding motifs to afford high-rate remediation nanocomposites, providing an excellent platform for next-generation arsenate remediation materials.