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Membranes 2022, 12, 343 16 of 27 physical contact of electrodes [102,103]. A typical CDI system is composed of a porous carbon electrode and a current collector. The surface of the CDI electrode may be further functionalized with specific chemical moieties or polymers to enhance ion selectivity [83,84]. The addition of ion-exchange species on porous electrodes enables selective ion capturing and prevents re-adsorption during the discharge of the electrode [80]. The nature of the functional groups located on the CDI scaffold affects the electrostatic interactions with ions [85,86], reduces energy requirements [87], and improves the process stability [85]. Coating of carbon electrodes with LiMn2O4 was performed to support Li recovery from lithium hydroxide solutions. The desorbed lithium ions from the modified MCDI system were found to be 8.7 mg/g at a constant voltage of 3.5 V, and this was lower (by approximately 45%) than the desorption for the conventional process with acidic solution [104]. A cathode composed only of LiMn2O4 was also developed [105]. The maximum salt adsorption capacity (SAC) was estimated at 24 mg of lithium per 1 g of electrode material. Moreover, this process did not require the use of the acidic solution in the desorption process [105]. Selective lithium recovery from multi-component aqueous solutions (Li+, Na+, K+, Ca2+, and Mg2+) reached 0.22 μg/g (with applied 1 V constant voltage electric mode) and was 7 times higher than that from a control physio-sorption process running (without application external electrical field) in similar experimental conditions during the CDI process. During application 1 V, the recovery amount of Li+ reached 350 μmol/gadsorbent. When the electrical field was not applied, the recovery reached only 50 μmol/gadsorbent. The energy required for the recovery was estimated to be 23.3 W h/g of lithium. Moreover, manganese dissolution was not observed during five consecutive recovery cycles support- ing the scalability and reproducibility of the process [106]. Monovalent selective cation exchange membranes (Neosepta CIMS, Astom Corporation, Japan) were tested for various rates of lithium over magnesium ions in feed solutions. The maximum performance was found to be 38.4% of recovered Li with an energy consumption 0.36 W h/g of lithium [107]. A hybrid capacitive deionization (HCDI) process has been performed with lithium titanium manganese oxide as the cathode material. The anode material was modified by adding polypyrrole (PPy) to increase the conductivity of the material. An electro-sorption capacity for LiCl of 36.9 mg/g was achieved while the corresponding capacities for NaCl and KCl were 18.09 mg/g and 9.07 mg/g, respectively [108]. Modified anion exchange membrane (AEM) was produced by chemical grafting of poly(vinyl chloride) (PVC) with aliphatic amines. The extraction of 40 mg/g of LiCl was obtained in comparison to 10 mg/g for NaCl. A recovery of about 50% of lithium was noted [94,109]. Poly(vinylidene fluoride) materials were evaluated as a supporting polymer for the AEM preparation. The salt adsorption capacity of the optimized materials was estimated at 30 mg/g with 0.9 current efficiencies and 96% of desorption efficiency [110]. The active cathode material is the next important element of the CDI system. Lithium– manganese–titanium oxide (LMTO) with varying concentrations of titanium dioxide (TiO2) has been tested as a cathode [98]. The best-performing material, which contained 5% of TiO2, had a sorption capacity of 36 mg/g, and the uptakes of KCl and NaCl were 16 and 11 mg/g, respectively. Additionally, this adsorbent needed two times less energy for the recovery of lithium chloride than other monovalent salts [98]. That adsorbent was used for selective recovery of Li from geothermal waters of the Western Carpathian Mountains region [7]. Lithium recovery of 73% was achieved with an extremely high salt adsorption capacity of 800 mg/g and total energy consumption of 0.183 W h/g [7]. Lithium–iron– manganese adsorbents, with varied ratios of Li/Mn and Li/Fe, were tested for a similar feed [101]. The adsorbents with the molar ratios of Li/Mn and Li/Fe of 1.5:1 showed the best salt adsorption capacity for LiCl. Moreover, 32 mg/g of lithium, 16 mg/g of sodium, and 0 mg/g of potassium was found. The use of a modified electrical protocol, with double stage of desorption, as found to be a good method for lithium recovery from solution. The recovery reached the efficiency of 76% and reduced the Na:K:Li-ions ratio from 227:1.1:1 at the feed to 2.9:0:1.PDF Image | Electro-Driven Materials and Processes for Lithium
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