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Acid baking treatment is widely used to extract rare earth elements (REEs) from refractory rare earth bearing minerals such as monazite and xenotime. Since these REE minerals have been identified in coal-based sources, a parametric study was conducted to evaluate the impact and optimize the parametric values associated with the acid-baking process when treating a bituminous coal source. The parameters studied using a three-level statistical experimental program were acid baking time, acid solution concentration, baking temperature, and acid solution-to-solids ratio and each were found to significantly impact REE and contaminant element recovery. An increase in baking temperature up to aroundmore » 250°C improved the light and heavy REE recovery values by more than 50 absolute percentage points relative to performances achieved when direct leaching. Acid baking was needed to dehydroxylate the clays and liberate the REE minerals, which allowed access for the acid to solubilize the REEs. Acid concentration of the solution used for acid baking was studied as a means of minimizing the amount of acid needed to achieve a target REE recovery. However, thermo-gravimetric and differential scanning calorimetry analysis (TGA-DSC) of sulfuric acid under oxidizing atmosphere revealed that the addition of water decreased the evaporation temperature, which explains the lower REE recovery values obtained when using lower acid concentrations. Using pure sulfuric acid at an acid-to-solid ratio of 0.8:1 resulted in recovery values of around 70% for both LREEs and HREEs. The decomposition reaction time was relatively quick with 65% of the TREEs recovered within the first 10 minutes. Water leaching experiments performed on the acid-baked products under a temperature of 25°C instead of 75°C revealed an increase in REE recovery by 10 absolute percentage points, which was likely due to the high solubility of REE-sulfates at room temperatures.« less

The recovery of rare earth elements (REEs) from secondary resources, particularly coal-based materials, has recently received attention due to supply and demand imbalance. Research reported to date indicates that a high REE recovery can be realized when treating bituminous coal sources using strong acid solutions of approximately100 g/L or higher. This study introduces an approach to enhance the total rare earth recovery (TREE), especially for heavy rare earth elements (HREEs), from these coal sources at significantly lower acid concentrations. Based on the presence of REE minerals like monazite and xenotime, a detailed investigation was undertaken to quantify three pre-leach treatmentmore » methods, i.e., 1) roasting, 2) direct acid baking, and 3) acid baking after roasting. Roasting tests at 600°C revealed that the recovery of light REEs (LREEs) was enhanced while the recovery of HREEs remained relatively unaffected. LREE and HREE recovery values of 38.3% and 21.3%, respectively, were achieved using a 50 g/L (0.5 M) sulfuric acid solution at 5% solid concentration and a solution temperature of 75°C for 2 h. Comparatively, direct acid baking at 250°C provided substantial increases in LREE and HREE recovery values to approximately 49.4% and 53.0%, respectively, using an equivalent acid dosage. Recoveries were maximized to 77.0% and 79.6% for LREE and HREE, respectively, by roasting followed by acid baking. Similar results were obtained from the treatment of a second bituminous coal source. Due to strong correlations between REE and Al recovery values, tests were performed on kaolinite and illite, which were prominent clay minerals within the source coals. In conclusion, these experiments revealed that the REE recovery improvements were likely a result of dehydroxylation of clays and subsequent release and decomposition of REE-bearing minerals such as monazite, xenotime and zircon.« less

Oxalic acid precipitation is a common step in the purification of rare earth elements (REE) from a concentrated pregnant leach solution (PLS). However, the presence of contaminants such as Al, Fe, and Ca in given amounts decreases the REE precipitation efficiency and product purity while also increasing the amount of oxalic acid needed to maximize recovery. As such, a statistically designed test program was performed to identify the optimal conditions necessary for a relatively low REE content PLS containing elevated concentrations of contaminant ions. The performance objective was maximization of REE precipitation efficiency while minimizing the oxalic acid dosage. Amore » central composite design was utilized to quantify performance impacts and identify the ultimate set of parameter values for oxalic acid dosage, Fe(III) contamination concentration, solution pH, and reaction temperature. The resultant model suggested that oxalic acid dosage and reaction pH are the most significant factors for the REE precipitation efficiency, followed by the interaction of oxalic dosage and Fe concentration. Test results indicate that increasing the oxalic acid concentration from 0 g/L to 80 g/L improved the REE precipitation efficiency from approximately 4.2% to 95.0%. Furthermore, raising the solution pH from 0.5 to 2.5 considerably enhanced the precipitation efficiency from 0.0% to 98.9%. A solution temperature elevation decreased REE recovery, which indicated an exothermic reaction between REEs and oxalate anions. Finally, a high level of Fe contamination adversely impacted REE precipitation efficiency. Here, to further the understanding of the REE-oxalate system, a fundamental solution chemistry study was performed using the equilibrium constants of the reactions. The study resulted in the development of oxalate speciation diagrams and provided an analysis of the REE precipitation characteristics at various oxalate anion concentrations and Fe(III) contamination levels using MINTEQ software. The dominant Fe(III) species in the solution system were found to be Fe-(C₂O₄)₃^3-, Fe-(C₂O₄)^2-, and Fe-(C₂O₄)⁺, which consume the majority of the oxalate anions. The simulated model was found to be in agreement with the experimental findings and helped to explain the adverse impact of increased iron concentrations on REE precipitation efficiency.« less

Recovery of rare earth elements (REEs) from coal samples collected from the Fire Clay coal seam using diluted mineral acid solutions was investigated. The initial processing step was coal recovery using conventional froth flotation which concentrated the REEs in tailing material resulting in an upgrade to values around 700 ppm on a dry whole mass basis. Leaching experiments were performed on the flotation tailings material using a 1.2 M sulfuric acid solution adjusted to a temperature of 75 °C to study the extractability of REEs from coal material. The effect of particle size, leaching time, leaching temperature, and solid concentrationmore » on REE leaching recovery were evaluated. The kinetic data obtained from leaching over a range of temperatures suggested that the leaching process follows the shrinking core model with possibly a mixed control mechanism that may be a result of several heterogenous materials leaching simultaneously. Leaching recovery increased rapidly at the beginning of the reaction then slowed as the system reached equilibrium. The apparent activation energy determined from test data obtained over a range of temperatures using 1 M sulfuric acid was 36 kJ/mol for the first 20 min of reaction time and 27 kJ/mol for the leaching period between 20 and 120 min. The leaching of light REEs during the initial stage was determined to be driven by a chemical reaction, followed by the formation of a product layer, which required lower activation energy in the later stage of leaching. In regards to the heavy REEs, the major mechanism for leaching is desorption and the product layer formation does not affect the heavy REEs significantly.« less

Photovoltaic (PV) technology offers an economic and sustainable solution to the challenge of increasing energy demand in times of global warming. The world PV market is currently dominated by the homo-junction crystalline silicon (c-Si) PV technology based on high temperature diffused p-n junctions, featuring a low power conversion efficiency (PCE). Recent years have seen the successful development of Si heterojunction technologies, boosting the PCE of c-Si solar cells over 26%. This article reviews the development status of high-efficiency c-Si heterojunction solar cells, from the materials to devices, mainly including hydrogenated amorphous silicon (a-Si:H) based silicon heterojunction technology, polycrystalline silicon (poly-Si)more » based carrier selective passivating contact technology, metal compounds and organic materials based dopant-free passivating contact technology. The application of silicon heterojunction solar cells for ultra-high efficiency perovskite/c-Si and III-V/c-Si tandem devices is also reviewed. In the last, the perspective, challenge and potential solutions of silicon heterojunction solar cells, as well as the tandem solar cells are discussed.« less

Lithium recovery from the density fractions of Baker (namely West Kentucky No. 13) seam coal was investigated in this study. Proximate and elemental analyses showed that lithium contents in the 1.8–2.2 SG and 2.2 SG sink fractions were 185 ppm and 150 ppm, respectively, which are significantly higher than the average content of coal sources (12 ppm) and coal ashes (66 ppm) worldwide. Moreover, due to the high lithium contents and mass distribution, nearly 90% of the lithium present in the Baker coal sample was distributed in the two density fractions. Direct leaching using a HCl solution resulted in lessmore » than 10% lithium recovery, which was due to nearly 90% of the lithium being associated with insoluble solids as determined by the results from sequential extraction tests. Calcination of both density fractions under 600 °C for two hours followed by leaching resulted in recovery increases in the range of 70% to 80%. The pyro-metallurgical pretreatment step converted most of the associated lithium minerals to more easy-to-leach forms such as carbonate and metal oxide. Based on mineralogy characterization and leaching test results, it was concluded that the positive effects of calcination on lithium leachability resulted from the dehydration and disintegration of kaolinite as well as dehydroxylation and expansion of muscovite/illite. Furthermore, an analysis of the leaching kinetics revealed that the leaching rate of lithium was controlled by interface transfer and diffusion across the product layer and was negatively impacted when the calcination temperature exceeded 600 °C due to sintering of the kaolinite.« less

Carrier-selective contacts have become a prominent path forward toward efficient crystalline silicon (c-Si) photovoltaics. Among the proposed contacting materials, organic materials may offer simplified and low-cost processing compared with typical vacuum deposition techniques. In this paper, branched polyethylenimine (b-PEI) is presented as an electron-transport layer (ETL) for c-Si solar cells. The incorporation of a b-PEI interlayer between c-Si(n) and Al leads to a low contact resistivity of 24 mΩ cm². A silicon heterojunction solar cell integrated with b-PEI is demonstrated achieving a power conversion efficiency of 19.4%, which improves the benchmark efficiency of a c-Si solar cell with an organicmore » ETL. This electron selectivity of b-PEI is attributed to its Lewis basicity, i.e., electron-donating ability, promoting favorable band bending at the c-Si surface for electron transport. Moreover, several other Lewis base polymers perform as efficient ETLs in organic/c-Si hybrid devices, indicating Lewis basicity could be a guideline for future organic ETL design.« less

The global photovoltaic (PV) market is dominated by crystalline silicon (c-Si) based technologies with heavily doped, directly metallized contacts. Recombination of photo-generated electrons and holes at the contact regions is increasingly constraining the power conversion efficiencies of these devices as other performance-limiting energy losses are overcome. To move forward, c-Si PV technologies must implement alternative contacting approaches. Passivating contacts, which incorporate thin films within the contact structure that simultaneously supress recombination and promote charge-carrier selectivity, are a promising next step for the mainstream c-Si PV industry. Here, we review the fundamental physical processes governing contact formation in c-Si. In doingmore » so we identify the role passivating contacts play in increasing c-Si solar cell efficiencies beyond the limitations imposed by heavy doping and direct metallization. Strategies towards the implementation of passivating contacts in industrial environments are discussed.« less

The majority of rare earth elements (REEs) existing in the feed to coal preparation plants report to the coarse refuse streams which are transported for permanent storage in contained piles. In this study, an integrated flowsheet was developed based on laboratory test data which combines physical separation, pyrite bio-oxidization, heap leaching, selective precipitation and solvent extraction processes. The test data was obtained from (1) characterization of a number of natural leachate and solid samples collected from different preparation plants which process coals from a number of coal seams and (2) laboratory acid leaching and selective precipitation tests results. The highly-valuedmore » critical REEs (i.e., Y, Nd, Eu, Tb and Dy) were selectively leached from the refuse samples in the natural environment due to the acid generated by pyrite oxidization. The leachate samples were evaporated to remove water and obtain residual solids (i.e., dissolved solids in the leachates). The total REE content in the dissolved solids from a given leachate sample was 380 ppm, which was higher than the REE content of the coarse refuse material that generated the leachate (322 ppm). Acid leaching tests recovered as much as 80% of the total REEs from the coarse refuse samples using a 1.2M sulfuric acid solution. Afterwards, the pH of the leachate was increased in a step-wise fashion which resulted in the production of precipitates containing 0.3–1.1% total REEs. A significant amount of contaminants, such as Fe, Al, and Ca, were eliminated in the sequential precipitation process, which allowed further upgrading using oxalic acid precipitation and/or solvent extraction. In the proposed flowsheet, the coarse refuse is arranged in heap leach pads and the acid needed for REE leaching is primarily produced from pyrite bio-oxidization, which enhances the selectivity of REE recovery and significantly reduces the cost. Furthermore, the successful application of the flowsheet would result in significant benefits to both the coal and rare earth industries.« less