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Membranes 2021, 11, 175 16 of 20 heat (e.g., 60 ◦C) can be utilized. In this work, we have simulated a three-stage lithium recovery process including the brine softening by precipitation Ca2+/Mg2+ cations with sodium carbonate (calculated in PHREEQC), followed by an integrated system consist- ing of membrane distillation unit (water evaporation), crystallizer (NaCl precipitation), and membrane extraction (Li+ recovery), which was simulated in Simulink/MATLAB. Simulink/MATLAB allows for simulating the operation of different units integrated into one system in the real-time regime. The small membrane surface area of 2.5 m2 for the integrated system of 140 kg of saline solution was selected to accumulate a sufficient number of membrane replacements within two months of operation for the evaluation. Based on the obtained results, the following conclusions and comments can be made: 1. High robust, fouling resistance membranes are needed. The deterioration of mem- brane performance in time due to scaling/fouling plays a critical role in the performance of the system. For example, if the membranes undergo greater irreversible fouling resulting in the recovery ratio of water flux after its washing every 4.5 h at 95% from the previous value instead of 99%, then two months of operation would require 21 replacements of membrane modules instead of 4. The specific lithium recovery per square meter of membrane in the module is mainly determined by the recovery ratio, which defines the lifetime of the membrane module, rather than the run time of the module before washing. 2. Low cost membranes are required. The process simulation based on the experi- mental and literature data on the high salinity solutions with the membrane distillation revealed that the specific productivity is within the range of 9.9–880 g(Li+) per square meter of membranes in the module used before the replacement, which makes 0.053–4.7 kg in the form of lithium carbonate or 0.5-42 USD (lithium carbonate price—58.5 CNY/kg at China Spot on 18.02.2021). However, all direct and indirect costs must be accounted; for instance, the microfiltration, hydrophobic membrane MFFK-1 used in this study to carry out the membrane distillation experiments costs 1300 Rub/m2 (~17.5 USD/m2). 3. The increase of energy efficiency is needed. The mass-flow-rate of saline solution circulated to the crystallizer was set at its almost minimum value as 6.5 kg/min to enable its successful operation at the given parameters of the membrane distillation unit. In other words, the operation of the integrated system having 140 kg of saline solution in the loop, membrane module of 2.5 m2 for concentration of lithium presence from 0.11 up to 2.3 g/kg would be associated with the circulation of about of 259 tons of saline solution per month between the distillation unit (60 ◦C) and the crystallizer (15 ◦C) to a yield of up to 1.4 kg of lithium ions. Therefore, it will be critical to implement the effective heat recuperation, which will be complicated by the fact that the saline solution is near saturation or oversaturation with regard to its temperature. 4. To increase the attractiveness of the geothermal brines as an alternative lithium source, novel concentration methods of high saline solutions with high robustness to the scaling and fouling during the long-term operation are needed. For instance, the thin- film distillation coupled with membrane condenser for brine solutions concentration was recently proposed [47]. In addition, lower temperature difference between different units of the integrated system might overcome the problem of salt precipitation and enable more effective heat recuperation. Supplementary Materials: The following are available online at https://www.mdpi.com/2077-037 5/11/3/175/s1, Supplementary S1: PHREEQC code for conversion the concentration from g/L to molality; Supplementary S2: PHREEQC code for simulation of CaCO3 and MgCO3 precipitation by Na2CO3. Boron was added with Na2CO3 in trace amounts to use it as a marker to draw a graph; Figure S1: Overview of the model in Simulink; Figure S2: Heater system in terms of Simulink; Figure S3: Crystallizer system in terms of Simulink; Figure S4: Crystallizer subsystem in terms of Simulink; Figure S5: Extractor system in terms of Simulink; Figure S6: Extractor subsystem in terms of Simulink; Figure S7: Membrane module system in terms of Simulink. Figure S8: Membrane fouling simulation system in terms of Simulink; Figure S9: Make-up flow system in terms of Simulink; Figure S10: Second heater subsystem in terms of Simulink; Figure S11: Subsystem for automatic calculation of the total membrane surface area in terms of Simulink.PDF Image | Process of Lithium Recovery from Geothermal Brine
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