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The 2060 Ma old Palabora Carbonatite Complex (PCC), South Africa, comprises diverse REE mineral assemblages formed during different stages and reflects an outstanding instance to understand the evolution of a carbonatite-related REE mineralization from orthomagmatic to late-magmatic stages and their secondary post-magmatic overprint. The 10 rare earth element minerals monazite, REE-F-carbonates (bastnasite, parisite, synchysite), ancylite, britholite, cordylite, fergusonite, REE-Ti-betafite, and anzaite are texturally described and related to the evolutionary stages of the PCC. The identification of the latter five REE minerals during this study represents their first described occurrences in the PCC as well as in a carbonatite complex in South Africa.The variable REE mineral assemblages reflect a multi-stage origin: (1) fergusonite and REE-Ti-betafite occur as inclusions in primary magnetite. Bastnasite is enclosed in primary calcite and dolomite. These three REE minerals are interpreted as orthomagmatic crystallization products. (2) The most common REE minerals are monazite replacing primary apatite, and britholite texturally related to the serpentinization of forsterite or the replacement of forsterite by chondrodite. Textural relationships suggest that these two REE-minerals precipitated from internally derived late-magmatic to hydrothermal fluids. Their presence seems to be locally controlled by favorable chemical conditions (e.g., presence of precursor minerals that contributed the necessary anions and/or cations for their formation). (3) Late-stage (post-magmatic) REE minerals include ancylite and cordylite replacing primary magmatic REE-Sr-carbonates, anzaite associated with the dissolution of ilmenite, and secondary REE-F-carbonates. The formation of these post-magmatic REE minerals depends on the local availability of a fluid, whose composition is at least partly controlled by the dissolution of primary minerals (e.g., REE-fluorocarbonates).This multi-stage REE mineralization reflects the interplay of magmatic differentiation, destabilization of early magmatic minerals during subsequent evolutionary stages of the carbonatitic system, and late-stage fluid-induced remobilization and re-/precipitation of precursor REE minerals. Based on our findings, the Palabora Carbonatite Complex experienced at least two successive stages of intense fluid-rock interaction.

In this paper, methods of effective removal of fluorine from rare earth chloride solution by adsorption, ion exchange and precipitation with lanthanum carbonate or CO2 gas as fluorine-removal agent, respectively, were studied. The relevant parameters studied for fluorine-removal percentage were the effects of the type and dosage of fluorine-removal agent, the injection flow and mode of CO2, the initial concentration of rare earth solution and initial pH value, contact time, temperature and stirring. XRD, SEM and EDS were used to analyze and characterize the filter slag obtained after fluorine removal. SEM and EDS results showed that RECO3(OH) with a porous structure was formed in rare earth chloride solution when lanthanum carbonate was used as fluorine-removal agent, and it had strong selective adsorption for F−. The XRD spectra showed that F− was removed in the form of REFCO3 precipitates, which indicates that the adsorbed F− replaced the OH− group on the surface of RECO3(OH) by ion exchange. The experimental results showed that a fluorine-removal percentage of 99.60% could be obtained under the following conditions: lanthanum carbonate dosage, 8%; initial conc. of rare earths, 240 g/L; initial pH, 1; reaction temperature, 90 ∘C; reaction time, 2 h. Simultaneously, a fluorine-removal process by CO2 precipitation was explored. In general, RE2(CO3)3 precipitation is generated when CO2 is injected into a rare earth chloride solution. Interestingly, the results of XRD, SEM and EDS showed that the sedimentation slag was composed of REFCO3 and RE2O2CO3. It was inferred that RE2(CO3)3 obtained at the initial reaction stage had a certain adsorption effect on F− in the solution, and then F− replaced CO32− on the surface of RE2(CO3)3 by ion exchange. Therefore, F− was finally removed by the high crystallization of REFCO3 precipitation, and excess RE2(CO3)3 was aged to precipitate RE2O2CO3. The fluorine-removal percentage can reach 98.92% with CO2 precipitation under the following conditions: venturi jet; CO2 injection flow, 1000 L/h; reaction temperature, 70 ∘C; initial pH, 1; reaction time, 1.5 h; initial conc. of rare earths, 240–300 g/L; without stirring. The above two methods achieve deep removal of fluorine in mixed fluorine-bearing rare earth chloride solution by exchanging different ionic groups. The negative influence of fluorine on subsequent rare earth extraction separation is eliminated. This technology is of great practical significance for the further development of the rare earth metallurgy industry and the protection of the environment.