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membranes Article A Comprehensive Membrane Process for Preparing Lithium Carbonate from High Mg/Li Brine Wenhua Xu, Dongfu Liu, Lihua He * and Zhongwei Zhao * School of Metallurgy and Environment, Central South University, Changsha 410083, China; xuwenhua@csu.edu.cn (W.X.); liudongfu@csu.edu.cn (D.L.) * Correspondence: helihua@csu.edu.cn (L.H.); zhaozw@csu.edu.cn (Z.Z.) Received: 21 October 2020; Accepted: 18 November 2020; Published: 26 November 2020 Abstract: The preparation of Li2CO3 from brine with a high mass ratio of Mg/Li is a worldwide technology problem. Membrane separation is considered as a green and efficient method. In this paper, a comprehensive Li2CO3 preparation process, which involves electrochemical intercalation-deintercalation, nanofiltration, reverse osmosis, evaporation, and precipitation, was constructed. Concretely, the electrochemical intercalation-deintercalation method shows excellent separation performance of lithium and magnesium, and the mass ratio of Mg/Li decreased from the initial 58.5 in the brine to 0.93 in the obtained lithium-containing anolyte. Subsequently, the purification and concentration are performed based on nanofiltration and reverse osmosis technologies, which remove mass magnesium and enrich lithium, respectively. After further evaporation and purification, industrial-grade Li2CO3 can be prepared directly. The direct recovery of lithium from the high Mg/Li brine to the production of Li2CO3 can reach 68.7%, considering that most of the solutions are cycled in the system, the total recovery of lithium will be greater than 85%. In general, this new integrated lithium extraction system provides a new perspective for preparing lithium carbonate from high Mg/Li brine. Keywords: membrane process; Li2CO3; electrochemical intercalation deintercalation; high Mg/Li brine 1. Introduction The fast development of electric vehicles, storage devices, and hand-held electronic devices has dramatically increased the demands for lithium [1–4]. Lithium carbonate is an important raw material for preparing lithium-ion battery cathode materials [5]. In recent years, global lithium (Li) demand has reached 180,000 tons of lithium carbonate equivalent in 2015, with forecasts as high as 1.6 M tons by 2030 [6,7]. Nowadays, lithium resources mainly exist in solid ore (such as spodumene and lepidolite) and brine, and over 70% of exploitable lithium in the world existed in the brine [8,9]. Compared with the lithium extraction from these two kinds of resources, lithium extraction from brine is more effective, simpler, and cheaper [8]. Most lithium resources in continental brines are found in a small region in South America, often referred to as the “Lithium Triangle” [9,10]. A notable feature of brines in the “Lithium Triangle” region is the low mass ratio of Mg/Li. In contrast, the grade of brine in other regions is much worse. In China, the major lithium-containing brines are located in the Qinghai–Tibet plateau [8,11], and most of the lithium-containing brines in this area are mostly magnesium sulfate subtype [12]. A typical feature of magnesium sulfate subtype brines is the mass ratio of Mg/Li, which has a long span (from tens to hundreds, even more than 1000) [13]. Therefore, how to effectively realize the separation of magnesium and lithium is the key to produce Li2CO3 from high Mg/Li brines. Multifarious methods such as solvent extraction [14], membrane separation [15–17], adsorption [18,19], and electrochemical intercalation-deintercalation (EID) method [17,20–23] have been developed for Membranes 2020, 10, 371; doi:10.3390/membranes10120371 www.mdpi.com/journal/membranesPDF Image | Membrane Process for Preparing Lithium Carbonate
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