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Electrodialysis (ED) with ion-exchange membranes is a promising method for the extraction of phosphates from municipal and other wastewater in order to obtain cheap mineral fertilizers. Phosphorus is transported through an anion-exchange membrane (AEM) by anions of phosphoric acid. However, which phosphoric acid anions carry the phosphorus in the membrane and the boundary solution, that is, the mechanism of phosphorus transport, is not yet clear. Some authors report an unexpectedly low current efficiency of this process and high energy consumption. In this paper, we report the partial currents of H2PO4−, HPO42−, and PO43− through Neosepta AMX and Fujifilm AEM Type X membranes, as well as the partial currents of H2PO4− and H+ ions through a depleted diffusion layer of a 0.02 M NaH2PO4 feed solution measured as functions of the applied potential difference across the membrane under study. It was shown that the fraction of the current transported by anions through AEMs depend on the total current density/potential difference. This was due to the fact that the pH of the internal solution in the membrane increases with the growing current due to the increasing concentration polarization (a lower electrolyte concentration at the membrane surface leads to higher pH shift in the membrane). The HPO42− ions contributed to the charge transfer even when a low current passed through the membrane; with an increasing current, the contribution of the HPO42− ions grew, and when the current was about 2.5 ilimLev (ilimLev was the theoretical limiting current density), the PO43− ions started to carry the charge through the membrane. However, in the feed solution, the pH was 4.6 and only H2PO4− ions were present. When H2PO4− ions entered the membrane, a part of them transformed into doubly and triply charged anions; the H+ ions were released in this transformation and returned to the depleted diffusion layer. Thus, the phosphorus total flux, jP (equal to the sum of the fluxes of all phosphorus-bearing species) was limited by the H2PO4− transport from the bulk of feed solution to the membrane surface. The value of jP was close to ilimLev/F (F is the Faraday constant). A slight excess of jP over ilimLev/F was observed, which is due to the electroconvection and exaltation effects. The visualization showed that electroconvection in the studied systems was essentially weaker than in systems with strong electrolytes, such as NaCl.

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Bilayer ion-exchange membranes are mainly used for separating single and multiply charged ions. It is well known that in membranes in which the layers have different charges of the ionogenic groups of the matrix, the limiting current decreases, and the water splitting reaction accelerates in comparison with monolayer (isotropic) ion-exchange membranes. We study samples of bilayer ion-exchange membranes with very thin cation-exchange layers deposited on an anion-exchange membrane-substrate in this work. It was revealed that in bilayer membranes, the limiting current’s value is determined by the properties of a thin surface film (modifying layer). A linear regularity of the dependence of the non-equilibrium effective rate constant of the water-splitting reaction on the resistance of the bipolar region, which is valid for both bilayer and bipolar membranes, has been revealed. It is shown that the introduction of the catalyst significantly reduces the water-splitting voltage, but reduces the selectivity of the membrane. It is possible to regulate the fluxes of salt ions and water splitting products (hydrogen and hydroxyl ions) by changing the current density. Such an ability makes it possible to conduct a controlled process of desalting electrolytes with simultaneous pH adjustment.