Fabrication of nitrogen-doped graphene quantum dots hybrid membranes and its sorption for Cu(II), Co(II) and Pb(II) in mixed polymetallic solution

With the rapid development of new–energy batteries, heavy-metals pollution from spent batteries has drawn much attention. Various techniques are recently proposed to delete or eliminate such pollution. Among which, membrane sorption exhibits exceptional advantages for the separation of multi-metal solution. For such a purpose, nitrogen-doped graphene quantum dots (N-GQDs) hybrid membranes were fabricated via sol–gel technique and hydrothermal synthesis, in which the precursor powder of N-GQDs was obtained by the combination of urea (used as a nitrogen source) and citric acid (used as a carbon source). Subsequently, the N-GQDs precursor was mixed with silane and PVA to generate N-GQDs hybrid membranes (NHMs). Competitive sorption of Cu(II), Co(II) and Pb(II) in the mixed polymetallic solution, such as a mixed Cu(II), Co(II) and Pb(II) ternary solution, a mixed Cu(II), Pb(II), Ca(II), Co(II) and Cr(III) quintuple solution, was investigated. It indicated that Cu(II) sorption on NHMs had better selectivity in these mixed polymetallic solutions. Moreover, sorption mechanism of Cu(II), Co(II) and Pb(II) demonstrates that the sorption of NHMs for Cu(II) and Pb(II) abided by Elovich model, indicating the properties of heterogeneous chemisorption. Such a trend shows that the sorption via chemical process between the active sites on the top-layer of NHMs, and Cu(II) and Pb(II) is one of the dominant interfering factors. Desorption testing demonstrated that EDTA-2Na is a best de-sorbent for Cu(II) sorption on NHMs and the number of cycles of these membranes can reach up to 10 times. These findings suggest that NHMs can be used to adsorb Cu(II), Co(II) and Pb(II) from mixed polymetallic solution, indicating promising applications in the successive separation of wastewater containing multiple mixed toxic metals from spent new-energy batteries and other metal-containing wastewater.