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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Pore-Scale Dynamics of Liquid CO2–Water Displacement in 2D Axisymmetric Porous Micromodels Under Strong Drainage and Weak Imbibition Conditions: High-Speed μPIV Measurements

Resolving pore-scale transient flow dynamics is crucial to understanding the physics underlying multiphase flow in porous media and informing large-scale predictive models. Surface properties of the porous matrix play an important role in controlling such physics, yet interfacial mechanisms remain poorly understood, in part due to a lack of direct observations. This study reports on an experimental investigation of the pore-scale flow dynamics of liquid CO 2 and water in two-dimensional (2D) circular porous micromodels with different surface characteristics employing high-speed microscopic particle image velocimetry (μPIV). The design of the micromodel minimized side boundary effects due to the limited size of the domain. The high-speed μPIV technique resolved the spatial and temporal dynamics of multiphase flow of CO 2 and water under reservoir-relevant conditions, for both drainage and imbibition scenarios. When CO 2 displaced water in a hydrophilic micromodel (i.e., drainage), unstable capillary fingering occurred and the pore flow was dominated by successive pore-scale burst events (i.e., Haines jumps). When the same experiment was repeated in a nearly neutral wetting micromodel (i.e., weak imbibition), flow instability and fluctuations were virtually eliminated, leading to a more compact displacement pattern. Energy balance analysis indicates that the conversion efficiency between surface energy and external work is less than 30%, and that kinetic energy is a disproportionately smaller contributor to the energy budget. This is true even during a Haines jump event, which induces velocities typically two orders of magnitude higher than the bulk velocity. These novel measurements further enabled direct observations of the meniscus displacement, revealing a significant alteration of the pore filling mechanisms during drainage and imbibition. While the former typically featured burst events, which often occur only at one of the several throats connecting a pore, the latter is typically dominated by a cooperative filling mechanism involving simultaneous invasion of a pore from multiple throats. This cooperative filling mechanism leads to merging of two interfaces and releases surface energy, causing instantaneous high-speed events that are similar, yet fundamentally different from, burst events. Finally, pore-scale velocity fields were statistically analyzed to provide a quantitative measure of the role of capillary effects in these pore flows.

Li, Yaofa↗
DOE OSTI2020

A Model of Ice Wedge Polygon Drainage in Changing Arctic Terrain

As ice wedge degradation and the inundation of polygonal troughs become increasingly common processes across the Arctic, lateral export of water from polygonal soils may represent an important mechanism for the mobilization of dissolved organic carbon and other solutes. However, drainage from ice wedge polygons is poorly understood. We constructed a model which uses cross-sectional flow nets to define flow paths of meltwater through the active layer of an inundated low-centered polygon towards the trough. The model includes the effects of evaporation and simulates the depletion of ponded water in the polygon center during the thaw season. In most simulations, we discovered a strong hydrodynamic edge effect: only a small fraction of the polygon volume near the rim area is flushed by the drainage at relatively high velocities, suggesting that nearly all advective transport of solutes, heat, and soil particles is confined to this zone. Estimates of characteristic drainage times from the polygon center are consistent with published field observations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Metal (Fe, Cu, and As) transformation and association within secondary minerals in neutralized acid mine drainage characterized using X-ray absorption spectroscopy

The formation and transformation of secondary minerals in areas affected by neutralized acid mine drainage (AMD) determine the behavior of toxic elements. To better understand the binding form of toxic elements in the secondary minerals, we focused on the distribution of secondary precipitates and heavy metals in neutralized AMD near a typical Cu-polymetallic deposit located in central Tibet. Compared to background values, the average heavy metal (As, Cu, Co, Cu, Mo, Pb, and Zn) content is higher in sediments close to the neutralized AMD drain. X-ray absorption spectroscopy (XAS) characterization shows the Fe in the suspended particulate matter (SPM) first aggregate as small Fe(III) octahedra clusters and then precipitate as ferrihydrite along the river. The XAS results also show the by-products of neutralization-ferrihydrite and sulfate-are the primary forms of Fe and S in the sediments, respectively. Gypsum retains Cu in the sediments via structural fixation, surface adsorption, and surface coprecipitation. The difference of Cu-O coordination number between the SPM and the sediments reveals the Cu sulfate coprecipitation on the surface of gypsum accompanied by SPM transporting along the river. XAS results confirm that ferrihydrite act as an essential sink for heavy metals, especially As. As (III) mineral in the sediment near the neutralized AMD outfall is dissolved and oxidized to arsenate downstream, which then adsorb to ferrihydrite and/or form As(V)-Fe minerals along the river. Gypsum and ferrihydrite have the potential to release heavy metals with changes in water chemistry, which may pose a threat to the safety of drinking water for downstream residents. These results deepen the understanding of the influence of secondary minerals (especially gypsum and ferrihydrite) on the migration and transformation process of heavy metal pollutants in mine drainage system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Advanced Processing of Rare Earth Elements and Critical Minerals from Acid Mine Drainage Feedstocks

Ongoing work by the project team identified a process for extracting rare earths and critical mineral (REE/CM) concentrates from acid mine drainage from coal mines, a major stream pollutant. The process removes harmful metals and separates REE/CM into economically attractive concentrates. This project explored the processing of those concentrates into individually separated, high purity metals, suitable for domestic manufacturers. The team brought unique experience in working with AMD-based feedstocks since the inception of USDOE’s coal-based REE/CM program in 2016. The project team has pioneered the recovery of rare earth/critical minerals (REE/CM) from acid mine drainage (AMD). This environmentally beneficial strategy will incentivize AMD treatment while recovering materials critical to the Nation’s defense and advanced manufacturing industries. In addition, the project will investigate the co-production of five high purity CMs from AMD, namely Co, Mn, Li, Cr, Ge. This team’s upstream and midstream recovery and processing technology has been demonstrated at the continuous, small scale pilot scale. In conjunction with the West Virginia Department of Environmental Protection, the team is constructing a full-scale, integrated, 500 gpm AMD treatment plant coupled with an REE/CM facility that will produce 21 tons REE/CM per year. Commissioning is scheduled for September 2021. This will provide feedstock for the team’s proprietary downstream processes that met the project objective: production of individually separated, high purity (ISHP) REE/CM oxides and their further processing to elemental metals (REM). To facilitate entry into the U.S. market, we have teamed up with companies that would use our products to strengthen their domestic supply chains and grow REE/CM based manufacturing in the U.S. They include Rockwell Automation, Rivian, Endress+Hauser, Inc., Northrop Grumman and Hela Novel Metals.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2025

Enhancing 2D hydrodynamic flood models through machine learning and urban drainage integration

Two-dimensional hydrodynamic flood models are commonly employed for simulating flood extent and inundation depth. However, the influence of urban drainage network (UDN) is frequently overlooked in these models, potentially compromising their accuracy. Furthermore, the expensive computational costs and longer processing times make them challenging for large-scale hydrodynamic simulation. To address these challenges, this paper develops a machine learning (ML)-driven emulator for an open-source flood model, the Two-dimensional Runoff Inundation Toolkit for Operational Needs (TRITON). A TRITON-ML Emulator (TR-Emulator) that utilizes Convolutional Long Short-Term Memory is developed to capture the spatiotemporal features of flood events based on the outputs from TRITON. We further enhance the emulator by integrating UDN parameters (TR-UDN), such as the flow capacity of drainage pipes, pipe size, and pipe length, via an ML stacking technique to improve the water surface elevation (WSE) simulation. Hurricane Harvey 2017 in Houston, TX is used as the case study. We compare WSE results from TRITON, TR-Emulator, TR-UDN, and the United States Geological Survey (USGS) observations to evaluate the performance of these models. The results indicate that the TR-Emulator effectively replicates the WSE simulated by TRITON. Additionally, TR-UDN performs well in capturing WSE patterns and peak flows, aligning more closely with USGS observations, except in areas with milder slopes where conveyance discrepancies are observed. We further test the generalizability of our ML-based models using another smaller event. This paper shows that the TR-Emulator is effective for users and engineers to emulate a 2D hydrodynamic model, and the enhanced version of the TR-Emulator, TR-UDN, can be an efficient tool for predicting WSEs during urban flooding.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Wintertime Supraglacial Lake Drainage Cascade Triggers Large‐Scale Ice Flow Response in Greenland

Surface melt forces summertime ice-flow accelerations on glaciers and ice sheets. Here, we show that large meltwater-forced accelerations also occur during wintertime in Greenland. We document supraglacial lakes (SGLs) draining in cascades at unusually high elevation, causing an expansive flow acceleration over a ~5,200 km 2 region during winter. The three-component interferometric surface velocity field and decomposition modeling reveal the underlying flood propagation with unprecedented detail as it traveled over 160 km from the drainage site to the margin, providing novel constraints on subglacial water pathways, drainage morphology, and links with basal sliding. The triggering SGLs continuously grew over 40 years and suddenly released decades of stored meltwater, demonstrating surface melting can impact dynamics well beyond melt production. We show these events are likely common and thus their cumulative impact on dynamics should be further evaluated.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Modeling the Effects of Artificial Drainage on Agriculture-dominated Watersheds using a Fully Distributed Integrated Hydrology Model: Datasets, code, models files

This model-data archive is for a modeling study focused on the effects of artificial drainage on agriculture-dominated watersheds using a fully distributed integrated hydrology model. This study introduced a novel strategy to represent the effects of tile drains and agricultural ditches in a fully distributed basin-scale integrated hydrology model. The numerical experiments in this study reveal the effects of surface and subsurface drainage on various hydrological states and fluxes. The details about the datasets can be found in the "readme" document attached with the dataset.

Agricultural Watersheds↗
DOE OSTI2022

Partitioning behavior and mechanisms of rare earth elements during precipitation in acid mine drainage

Rare earth elements (REEs) are frequently found concentrated in acid mine drainage (AMD). The recovery of REEs from AMD has been successfully achieved using selective chemical precipitation. However, a portion of the REEs is often lost to the precipitates of the dominant metal contaminant ions. To better understand the REE partitioning behavior and mechanisms during the precipitation process, a systematic study was performed on both natural and synthetic AMD solutions. Precipitation test results show that REE removal was noticeably elevated at pH 4.0 after adding H 2 O 2 to convert ferrous to ferric ions, causing nearly complete precipitation of iron. Solution equilibrium calculations suggested that the REE removal increase was realized through adsorption onto the surfaces of the ferric precipitates. The presence of aluminum species in the solutions reduced the adsorption of REEs on the ferric precipitates. Based on electro-kinetic test results, it was concluded that aluminum species neutralize the negative surface charge of the ferric precipitates and compete with REEs for the adsorption active sites. The presence of ferrous ions in the solutions reduced REE adsorption on the aluminum precipitates at lower pH values (e.g., 5.0) due to competitive adsorption. However, at higher pH values (e.g., 6.0), REE removal to the precipitate product increased due to the precipitation of ferrous ions. Additionally, to the electro-kinetic tests and solution equilibrium calculations, mineralogy characterization, specific surface area measurement, particle size analysis, and morphology analysis were also conducted to investigate and identify the partitioning mechanisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Process development for recovering critical elements from acid mine drainage

The rapid development of advanced technologies has increased the demand for critical elements, such as Mn, Co, and Ni. For this work, a systematic study was conducted to develop a process for producing high-purity Mn, Co, and Ni products from an acid mine drainage (AMD). As major contaminants, Fe and Al in the solution were sequentially precipitated and eliminated by elevating the pH to around 4.00 and 6.50, respectively. After that, a pre-concentrated slurry containing 3,794 mg/L Mn, 59 mg/L Co, 127 mg/L Ni, and 300 mg/L Zn was obtained by collecting the precipitates formed in the pH range of 6.50 to 10.00. The pH of the pre-concentrated slurry was decreased to around 5.00 by adding HCl to re-dissolve Co, Ni, and Zn for further purification. At this pH, greater than 50% of Mn remained undissolved, and filtration of the undissolved material resulted in a product with around 30 wt.% Mn. Sodium sulfide was added into the re-dissolved solution to selectively precipitate Co, Ni, and Zn while remaining Mn in the solution. Almost 100% of Co, Ni, and Zn but only around 15% of Mn were precipitated using a sulfur to metal molar ratio of 1 at pH 4.00. The sulfide precipitate was calcined at 200 °C for 2 h and then completely dissolved in 1.2 M HCl. The critical elements existing in the dissolved solution were efficiently separated using a two-stage solvent extraction process. Ultimately, Co and Ni products with almost 94% and 100% purity were obtained by sulfide and alkaline precipitation, respectively.

42 ENGINEERING↗
DOE OSTI2022

Development of a chemical-free process utilizing ozone oxidative precipitation for the recovery of cobalt and manganese from acid mine drainage

Acid mine drainage (AMD) has been identified as a viable secondary resource of Co, and Mn. However, recovery of these elements while treating AMD is challenging due to the unfavorable pH and Eh conditions for Co-Mn precipitation. This study investigated the effects of various ligands (hydroxide, carbonate, ammonium, sulfate, and phosphate) and oxidizers (sodium persulfate, potassium permanganate, and ozone) on the precipitation of Co-Mn from AMD through experimental and solution chemistry studies. Ozone was found to be the most effective agent for the recovery of these elements. Based on the results, an AMD treatment process was formulated for selective recovery of multiple critical elements, including Al, REEs, Co, and Mn. More than 95 % of Co and Mn were recovered through the proposed process utilizing chemical-less ozone oxidative precipitation. In conclusion, a precipitate containing 0.9 % Co and 54.6 % Mn was obtained from an AMD source containing 0.9 ppm Co and 41.8 ppm Mn.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Technoeconomic Assessment of a Sequential Step-Leaching Process for Rare Earth Element Extraction from Acid Mine Drainage Precipitates

Herein, Coal waste products have been studied as a new source of Rare Earth Elements (REEs) and other Critical Minerals (CM) essential for the development of renewable energy technologies, but the economic viability of these source materials is not well understood. This paper examines the technoeconomic performance of a novel process for rare earth element extraction from acid mine drainage precipitates (AMDp) in the Appalachian Coal Basin. The three phase extraction process includes excavation and transportation of AMDp, multi-phase pH driven step-leaching of REEs at ambient conditions, and commercial solvent extraction to produce a saleable grade rare earth oxide material that can be reduced to a pure metal. We estimate the life-cycle cost of bench-scale extraction of REEs from two representative Appalachian AMDp feedstock chemistries at between 4000 – 6000 $/kg of mixed REE concentrate produced. Both the AMDp composition and process parameters affect the profitability of REE extraction, with the REE concentration and distribution of REE in the feedstock, extraction and precipitation reagent consumption rates, and the potential for reagent recycling as the key variables. Economically profitable valorization of REE from AMDp will require a combination of continued process innovation and sizable financial incentives to substantially influence domestic supply of REEs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Recovering Rare Earth Elements from Coal Mine Drainage Using Industrial Byproducts: Environmental and Economic Consequences

Coal mine drainage (CMD) impairs tens of thousands of kilometers of U.S. waterways each year, in part with the leaching of low concentrations of rare earth elements (REEs). REEs are essential for modern technologies, yet economically viable natural deposits are geospatially limited, thus engendering geopolitical concerns, and their mining is energy intense and environmentally destructive. This work summarizes laboratory-scale experimentalresults of a trap-extract-precipitate (TEP) process and uses the mass and energy balances to estimate the economic costs and environmental impacts of the TEP. The TEP process uses the alkalinity and filtering capacity of stabilized flue gas desulfurization (sFGD) material or water treatment plant (WTP) sludge to remediate CMD waters and extract REEs. Passive treatment systems that use WTP sludge are cheaper than those that use sFGD material ($\$$89,300/year or $\$$86/gT-REE vs. $\$$89,800/year or $\$$278/gT-REE) and have improved environmental performance across all indicators from two different impact assessment methods. These differences are largely attributable to the larger neutralizing capacity of WTP sludge in the treatment application.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2025

Assessing the Role of Hydrodynamics in Enhancing Height-Above-the-Nearest-Drainage Derived Synthetic Rating Curves: A Comparative Study in the Wu River Basin, Taiwan

The conventional approach to generating synthetic rating curves (SRC) using the Height-Above-the-Nearest-Drainage (HAND) method typically relies on the assumption of uniform flow, such as Manning's equation, to establish stage-discharge ratings. The zero-physics application of the uniform flow equation is insufficient for capturing detailed hydraulic features (e.g., backwater effect) and neglects the hydraulic effects from adjacent channels. This lack of hydrodynamic computation can impact the accuracy and effectiveness of riverine flood risk estimation and management. To reduce this foreseeable error, we introduce the HAND-hd workflow, which integrates sophisticated hydrodynamic computations in the production of HAND-based SRC with hydrodynamic features (SRC hd ). The results indicate that SRC hd demonstrates consistent agreement with both gauge observations and benchmark solutions. Additionally, the comparative analysis suggests that SRC hd provides notable improvements in stage-discharge ratings over conventional HAND-based SRCs, particularly in channels with mild bed gradients, where it reduces water stage prediction errors and percent biases. In steeper channel segments, SRC hd maintains comparable accuracy to conventional methods. The comprehensive evaluation in this study emphasizes the potential discrepancies and inaccuracies associated with the adoption of the uniform flow assumption in the conventional HAND-SRCs and addresses the necessity of including hydrodynamic physics in the application of HAND-based SRC (e.g., inundation map) in channels with mild gradients.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Bacterial nitrite production oxidizes Fe(II) bioremediating acidic abandoned coal mine drainage

Passive remediation systems (PRSs) treating either acidic or neutral abandoned coal mine drainage (AMD) are colonized by bacteria that can bioremediate iron (Fe) through chemical cycling. Due to the low pH in acidic AMD, iron oxidation from soluble Fe(II) to precipitated Fe(III) is mainly directed by microbial oxidation. Less well described are biotic reactions that lead to iron remediation through abiotic secondary reactions. We describe here iron oxidation in acidic AMD that is mediated by the bacterial reduction of nitrate to nitrite followed by the geochemical oxidation of Fe(II). Within an acidic PRS, 4,560 bacteria cultured from the microbial community were screened for their ability to oxidize iron and to perform nitrate-dependent iron oxidation (NDFO). Iron oxidation in the culturable community was observed in every pond of the system, ranging from 2.1% to 11.4%, and NDFO was observed in every pond, ranging from 1.4% to 6.0% of the culturable bacteria. Five NDFO isolates were purified and identified as Paraburkholderia spp. One of our isolates, Paraburkholderia sp. AV18 was shown to drive NDFO through the bacterial production of nitrite that in turn chemically oxidizes Fe(II) (nitrate reduction-iron oxidation; NRIO). AV18 expressed nitrate reductase, napA, concurrent to nitrite production. Burkholderiales are found by 16S rRNA gene sequencing in every pond of the PRS. The frequency of NDFO metabolism in the culturable microbial community and abundance of Burkholderiales in the PRS suggest nitrite producers contribute to the bioremediation of iron in acidic AMD and may be an unharnessed opportunity to increase iron bioremediation in acidic conditions.

(NDFO)↗
DOE OSTI2021

Concentrating Rare Earth Elements in Coal mine drainage Using Coal Combustion Products through Abandoned Mine Land Reclamation

Rare earth elements (REEs) (including scandium, yttrium and a group of 15 lanthanides) are often considered to be critical components in the productions of renewable energy hardware, electric vehicles, health care and military equipment, and consumer electronic products. The demand of REEs has been projected to be growing at an annual rate of 5-9% in the next 25 years. In 2011, the global demand of total rare earth oxides (REOs) was estimated to be approximately 105,000 tons, which is expected to grow to 210,000 tons by 2025. China overwhelmingly dominates the current worldwide rare earth productions but has strategically restricted its exports, causing significant instability for the global market. In response to the increasing demand for REEs and the supply dominance of China, identifying alternative sources of REEs has become a critical issue for the United States and other countries. Coal, coal ash, and coal mine drainage (CMD) are considered to be the alternative sources of REEs. In the U.S., high REE concentrations have been reported to be closely associated with coal deposits, including the Appalachian Basins. When surface and/or groundwater come in contact with geologic strata containing sulfide minerals exposed by coal mining, the accelerated oxidation of sulfide minerals in the presence of ferric iron and/or oxygen can produce sulfuric acid. The process promotes the weathering of REE-bearing rocks and minerals in the host geologic strata. Compared to average river water and seawater, the concentrations of REEs can be orders of magnitude higher in CMD. In this study, we demonstrated a trap-extract-precipitate (TEP) process that can effectively recover REEs from CMD. The three-stage TEP process uses alkaline industrial by-products to capture REEs from CMD and then applies an extraction/precipitation procedure to produce a feedstock that can be economically processed to produce marketable rare earth oxides. The alkaline industrial by-products tested in this study include the residual from a water softening process (DRWP sludge) and two types of stabilized flue gas desulfurization materials (sFGDs). sFGD material is a mixture of lime (CaO) and two coal combustion by-products, calcium sulfite FGD by-product and fly ash. The objectives of this study are to (1) validate the effectiveness and feasibility; (2) determine mechanisms controlling the rare earth recovery, (3) quantify the associated economic and environmental benefits, and (4) evaluate the full-scale application. To achieve these objectives, tasks to be carried out in this proposed project are organized into three phases. In the first phase, the research team collaborated with Ohio Department of Natural Resources, American Electric Power, The Wilds (a nonprofit wildlife conservation organization), and a private landowner to carry out field investigations aimed to screen and evaluate the seasonal changes of rare earths in the CMD discharges that have high recovery potentials. Next, the recovery of REEs from CMD was tested using a series of lab-scale column and batch tests under, respectively, percolation and completely mixed conditions. Results obtained from these lab-scale studies show that all three tested solids are very effective in retaining REEs. Over 98% of the CMD REEs that contacted the solids were captured before the solids exhausted their neutralization capacities. We also determined an extraction process using a non-acid, organic ligand extraction solution that can effectively remobilize the retained REEs from the spent solids (over 90%). The REE concentrate (>7.5 wt. % of total REEs) is then formed in an aeration process. The TEP process uses environmentally benign industrial by-products and a naturally-occurring organic ligand to mitigate CMD and recover REEs. Techno-economic analysis (TEA) and life-cycle assessment (LCA) was carried out in the third phase. The engineering-economic costs and net energy, net CO2 emissions, and water and other requirements were investigated to understand the economic and environmental implications of this process. This work uses mass and energy balances from laboratory-scale experiments to estimate the economic costs and environmental impacts. The results suggest that passive treatment systems that use DRWP sludge are preferred over those that use sFGD material, because of lower economic costs ($89,300/yr with a unit cost of $86/gT-REE vs. $89,800/yr, or $278/gT-REE) and improved environmental performance across all indicators from two different impact assessment methods. These differences are largely attributable to the larger capacity of DRWP sludge in the passive treatment application. We envision this TEP process can be integrated with abandoned mine land (AML) reclamation to create an approach that can add economic incentives for AML reclamation, remediate CMD discharge, and eliminate public safety hazards and threats to local environment and ecological systems posed by AMLs. It can restore lands and communities that are adversely impacted by legacy mining.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2024

Targeted Rare Earth Element Extraction from Mine Drainage Treatment Solids Informed by Advanced Characterization

In support of a clean energy transition in the U.S., National Energy Technology Laboratory (NETL) has collaborated with staff at Hedin Environmental and students at the University of Pittsburgh to characterize critical mineral content and recovery potential from acid mine drainage treatment solids (AMD solids). AMD solids in Appalachia are an unconventional feedstock of rare earth elements (REEs), with potential of suppling 1,102 tons REE/year. To inform recovery efforts, select AMD solids were examined using synchrotron microprobe analysis in conjunction with USGS-developed geochemical modeling to indicate likely phases hosting critical minerals (REE, Co, Ni, etc.) and associated metals . More than 100 AMD solids were collected from 94 passive AMD treatment systems in Pennsylvania, where limestone aggregates are used for acidity neutralization. As pH increases, dissolved metals and critical minerals in AMD are attenuated as surface coatings on limestone. The collected AMD solids contained up to 2000 mg/kg REE, up to 13,000 mg/kg transition metals (Co, Ni, Zn) and up to 440 mg/kg Li. Regardless of the diverse chemical compositions from AMD solids (Al-rich, Mn-rich, or Al,Fe,Mn-rich), REEs were mostly associated with Al and Mn (hydr)oxides, while select heavy REEs (e.g., Gd, Dy) were co-localized with Fe (hydr)oxides. Co and Ni have different distribution zones, while both co-localized with Mn (hydr)oxides. Based on this characterization, NETL developed a patent-pending innovative step-leaching protocol, “Targeted Rare Earth Extraction (TREE)” to effectively recover up to 90% REE and 60% Co in separate steps. In addition, select post-TREE solid residuals (purified Al oxides, or Mn oxides) can be further developed into functional materials (e.g., lithium and CO2 sorbents) needed for green energy transition and carbon management. This characterization-informed approach as well as TREE processing from AMD solids can be used for other legacy wastes (e.g., coal ash, oil and gas drill cutting, mine tailings), and offers an opportunity to transform waste streams into environmental and economic assets that meet U.S. Department of Energy and U.S. Environmental Protection Agency goals.

characterization and extraction of rare earth elem↗
DOE OSTI2021

A Fundamental Economic Assessment of Recovering Rare Earth Elements and Critical Minerals from Acid Mine Drainage Using a Network Sourcing Strategy

In recent years, acid mine drainage (AMD) has emerged as a promising unconventional source of rare earth elements (REEs) and other critical minerals (CMs) such as cobalt and manganese. In this regard, AMD provides a natural heap leaching effect that extracts and concentrates REE/CM from the host strata creating a partially enriched feedstock suitable for downstream extraction, separation, and recovery. While several prior studies have described processes and approaches for the valorization of AMD, very few have described the supply chain and infrastructure requirements as well as the associated economic assessment. To that end, this paper provides a fundamental economic assessment of REE/CM recovery from AMD using a network sourcing strategy in addition to a robust, flexible feedstock separations and refining facility. The methodology of this paper follows that of a typical techno-economic analysis with capital and operating costs estimated using AACE Class IV (FEL-2) guidelines. To demonstrate the range of possible outcomes, four pricing scenarios were modeled including contemporary prices (September, 2021) as well as the minimum and maximum prices over the last decade. In addition, five production scenarios were considered reflecting variations in the product suite, ranging from full elemental separation to magnet REE and CM production only (i.e., Pr, Nd, Tb, Dy, Y, Sc, Co, and Mn). The results of this analysis show that, with the exception of the minimum price scenario, all operational configurations have positive economic indicators with rates of return varying from 25% to 32% for the contemporary price scenario. The optimal configuration was determined to be production of Co, Mn, and all REEs except for mischmetal, which is not recovered. Sensitivity analysis and Monte Carlo simulation show that capital cost and HCl consumption are the two major factors influencing rate of return, thus indicating opportunities for future technology development and cost optimization. Implications of the study and a cooperative profit-sharing model for sourcing are also described.

42 ENGINEERING↗
DOE OSTI2022

A Hybrid Experimental and Theoretical Approach to Optimize Recovery of Rare Earth Elements from Acid Mine Drainage Precipitates by Oxalic Acid Precipitation

The development of processing techniques for the extraction of rare earth elements and critical minerals (REE/CM) from acid mine drainage precipitates (AMDp) has attracted increased interest in recent years. Processes under development often utilize a standard hydrometallurgical approach that includes leaching and solvent extraction followed by oxalic acid precipitation and calcination to produce a final rare earth oxide product. Impurities such as Ca, Al, Mn, Fe and Mg can be detrimental in the oxalate precipitation step and a survey of the literature showed limited data pertaining to the REE precipitation efficiency in solutions with high impurity concentrations. As such, a systematic laboratory-scale precipitation study was performed on a strip solution generated by the acid leaching and solvent extraction of an AMDp feedstock to identify the optimal processing conditions that maximize REE precipitation efficiency and product purity while minimizing the oxalic acid dosage. Given the unique chemical characteristics of AMDp, the feed solution utilized in this study contained a moderate concentration of REEs (440 mg/L) as well a significant concentration (>7000 mg/L total) of non-REE contaminants such as Ca, Al, Mn, Fe and Mg. Initially, a theoretical basis for the required oxalic acid dose, optimal pH and predicted precipitation efficiency was established by solution equilibrium calculations. Following the solution chemistry calculations, bench-scale precipitation experiments were conducted and these test results indicate that a pH of 1.5 to 2, a reaction time of more than 2 h and an oxalic acid dosage of 30 to 40 g/L optimized the REEs recovery of at ~95% to nearly 100% for individual REE species. The test results validated the optimal pH predicted by the solution chemistry calculations (1.5 to 5); however, the predicted dosage needed for complete REE recovery (10 g/L) was significantly lower than the experimentally-determined dosage of 30 to 40 g/L. The reason for this discrepancy was determined to be due to the large concentration of impurities and large number of potential metal complexes that cause inaccuracies in the solution equilibrium calculations. Based on these findings, a hybrid experimental and theoretical approach is proposed for future oxalic acid precipitation optimization studies.

oxalic acid precipitation↗