Preamble

Study Static Leaching Kinetics Uranium Tailings Multi-factor Interaction

Analysis

b,a,c* China Institute Radiation Protection, Laboratory Radiation Environment Health Ministry Ecology Environment, Taiyuan 030006, China Wuhan University Science Technology, School Resources Environmental Engineering, Wuhan 430081, China China Institute Radiation Protection, Laboratory Radiation Protection Technology Taiyuan 030006, China author.

School Resources Environmental Engineering, Wuhan University Science Technology, Wuhan, 421001, China. address:

Zhao).

Abstract

Uranium tailings harbor long-lived, highly biotoxic radionuclide alongside associated heavy metals, posing persistent environmental risks.

However, comprehensive systematic studies leaching mechanisms, kinetics, interaction environmental factors release under static conditions remain critically lacking. solve above problems, study, effects solid- liquid ratio, concentration, concentration leaching investigated using custom-designed static leaching device found lower reduced solid-to-liquid ratio, elevated concentration, higher concentration conducive enhanc leaching rates Mechanistic

analysis

reveals lower elevates leaching rates solution-phase concentrations through mineral disintegration, increased specific surface area, -competitive displacement lower solid-to-liquid ratio maintains higher diffusion driving force, enhancing interfacial contact solid leachant High-concentration disrupts lead-bearing mineral structures Strong oxidizing capacity, enhancing solubility altering surface properties promote desorption accelerates leaching -competitive exchange -assisted chelation dissolution. leaching kinetic model established based experimental effect two-factor interaction leaching quantified using Box-Behnken design soft, identifying parameter combinations maximal leaching rates.

These findings provide robust theoretical foundation predicting leaching migration hazardous elements uranium tailings under static aquatic environment eywords Migration Static Leaching Leaching Kinetics Interaction Uranium Tailings

1. Introduction

Uranium tailings, byproduct uranium mining milling operations, persistent environmental risks radionuclides uranium decay series co-occurring heavy metals (e.g., Abdelouas Stored hydrogeological systems, tailings

undergo continuous water-rock interactions. process governed mineral dissolution-precipitation equilibria, exchange, colloid transport Nordstrom, mobilize bound-phase heavy metals freely dissolved species, significantly elevating contaminant migration rates Martin Field studies decommissioned tailings ponds South China demonstrate precipitation-driven leachate release constitutes primary pathway radionuclide heavy metal dispersion surrounding aquifers soils Secondary pollution arising hydrogeochemical process represents critical challenge environmental remediation tailings sites Consequently, revealing release kinetics migration mechanisms pollutants uranium tailings under aqueous conditions significant theoretical importance advancing pollution prevention management decommissioned tailings facilities. recent years, research pollutant release mechanisms uranium tailings predominantly focused hydrogeochemical behavior dynamic migration patterns major radionuclides Martin 2003; Within uranium decay chain, radionuclide exhibits complex leaching mechanisms half-life (22.3 years), biotoxicity, intricate occurrence characteristics tailings-water interface.

Current studies leaching primarily investigate behavior soils, concentrating effects leachate organic chelating agents (citric polyepoxysuccinic oxalic inorganic stabilizing materials (phosphates Fayiga apatite zeolite properties (organic matter content Chamorro nchez-Andica compaction Research specifically targeting leaching uranium tailings remains limited, having addressed influence through column leaching experiments simulating rainwater percolation through uranium tailings varying levels, demonstrated leaching dissolution-controlled, lower enhancing migration conducting static leaching experiments uranium tailings under different conditions, concluded primarily influences leaching altering chemical speciation 210Pb physicochemical properties tailings particles However, leaching behavior mechanisms 210Pb under static immersion conditions, leaching kinetics, interactive effects critical environmental factors leaching rates still systematic in-depth investigation. elucidate static leaching behavior uranium tailings under natural precipitation, study systematically investigated leaching characteristics kinetics using fresh uranium tailings samples under various influencing factors.

Single-factor influence experiments conducted custom-designed static leaching device investigate leaching behavior mechanisms Subsequently, leaching kinetics

analysis

performed based experimental

results

establish leaching kinetics model Finally, response surface

methodology

applied study interactive effects environmental factors leaching identify critical parameters achieving maximum leaching research provides theoretical basis revealing leaching migration behavior harmful metal elements uranium tailings under static water immersion conditions.

Experiments Experimental Materials Samples tailings tailings impermeable layer

selected. After air-drying, tailings samples subjected sample reduction quartering method.

Mineral composition trace element

analysis

performed representative specimens using X-ray diffraction (XRD),

results

presented Tables shown Table tailings predominantly composed quartz 50%), while consists mainly gypsum 40%).

Table indicates uranium content tailings thorium content values significantly exceeding average concentrations (3.08 (15.4 g/g). samples subjected sequential extraction, speciation presented Table mobile fraction constitutes 22.2%.

Table Mineral composition uranium tailings samples

Mineral component Quartz Plagioclase K-feldspar Illite Kaolinite Gypsum

tailings Element Water-soluble Exchangeable Carbonate-bound Fe-Mn oxide-bound Organic matter-bound Residual

2.2 Experimental

device custom-designed static leaching device employed, structure illustrated Figure device measures length, width, height. partition installed along length device prevent tailings particles entrainment during supernatant withdrawal. upper portion partition features multiple small apertures facilitate solution diffusion sides.

Additionally, ventilation apertures device allow creation aerobic anaerobic leaching conditions. internal structure diagram physical object photograph

2.3 Experimental

protocol Effect different values: Solutions values accurately prepared dropwise addition solutions container.

Subsequently, tailings (particle size: placed static leaching device, prepared solution added.

After standing period, radionuclide

concentrations supernatant measured determine effects different values leaching durations.

Effect different solid-to-liquid ratios: Tailings particle selected. tailings placed separate static leaching devices, deionized water added each.

After standing period, radionuclide concentrations supernatant measured determine effects different leaching durations solid-to-liquid ratios 1:10, 1:20, 1:30, 1:40.

Effect different oxidizing conditions: tailings particles placed separate static leaching devices, solutions concentrations mol/L, mol/L, mol/L, mol/L added each. adjusted After standing period, radionuclide concentrations supernatant measured determine effects different leaching durations under different oxidizing conditions.

Effect Different Ionic Strengths: 100-g tailings particles placed separate static leaching devices, solutions concentrations mol/L, mol/L, mol/L added each. adjusted After standing period, radionuclide concentrations supernatant measured determine effects different leaching durations different ionic strengths.

Results

Effect variation activity concentration leachate leaching illustrated curve variation indicate that, under varying conditions, activity concentration solution undergoes three distinct stages: rapid leaching, leaching, leaching equilibrium. identical leaching times, higher value corresponds lower activity concentration solution, activity concentration being significantly greater demonstrates increase value

results

decreased leaching equilibrium. Comparative

analysis

Figs. reveals lower solution yields higher leaching concentration, shorter duration attain leaching equilibrium, greater favorability leaching. further elucidate experimental causation, chemical speciation leachate characterization leached residue analyzed. depicted percentage variations demonstrate predominantly exists between precipitates gradually becomes dominant solid phase; between emerges predominant precipitate phase; between Pb(OH) serves primary precipitate phase, further inhibiting release. image post-leaching uranium tailings residue (Fig. reveals tailings exhibit fragmented morphology well-developed microporosity, enhancing solid-liquid contact facilitating leaching. increasing tailings consolidation intensifies, accompanied micropore closure, which impedes solution penetration diffusion. evidenced Figs. concentration variations Figs. arise following mechanisms. strongly acidic environment promotes -driven erosion lead-bearing minerals, dissolving carbonate oxide cementing agents causing tailings disintegration fragments. increases specific surface tailings opens diffusion channels.

Concurrently, competes adsorption sites,

concentrations occupying surface sites tailings inducing desorption bound thereby accelerating release acidic environment facilitates -mediated sulfate dissolution tailings, generating which combines low-solubility thereby reducing aqueous concentration. leaching governed combined kinetics dissolution precipitation alkaline environment drives -induced carbonate mineral dissolution, elevating concentration forming which lower solubility precipitate further clogs tailings micropores covers active sites mineral surfaces, impeding solution contact unreacted minerals. conditional solubility product Pb(OH) reaches minimum, minimizing solubility; concentrations induce gel-like coagulation Pb(OH) exacerbating cementation leaching activity concentration leachate function leaching leaching equilibrium

( c ) Chemical speciation of 210 Pb under varying initial pH conditions of leachate

Effect leaching

SEM images of uranium tailings under varying pH conditions.

Effect Solid-to-Liquid Ratio Figure shows leaching behavior under varying solid-to-liquid ratios. shown Figure increasing leaching time, 210Pb activity concentration solution shows rapid increase increase equilibrium attributed dominance readily accessible soluble particle surfaces during where dissolution rates governed surface chemical reaction kinetics, resulting rapid concentration increase During after depletion surface-soluble components, leachate diffuses solid interior react, resulting

210 Pb

diffuse internal pores lattices particle surfaces, dissolution rates controlled solid-phase diffusion transfer, significantly slowing process During leached quantity approaches maximum solubility achievable under given solid-to-liquid ratio, reaching dissolution equilibrium. leaching solid-to-liquid ratio Variation activity concentration leaching time; Variation leaching uranium tailings Leaching behavior under different solid- liquid ratios. leaching efficiency.

Comparing Figures reveals higher solid-to-liquid ratio increases concentration decreases leaching efficiency. occurs because higher ratio indicates solid particles solution volume, which elevates total dissolved time. concentrations reduce concentration gradient between particle surfaces solution, inhibiting diffusion causing incomplete dissolution.

Concurrently, reduced leachate volume solid promotes local saturation particles, hindering further dissolution internal lowering leaching efficiency Conversely, lower ratio corresponds fewer solids volume, reducing total dissolution

maintaining lower concentration gradient. low-concentration environment sustains diffusional driving force, enabling complete reaction. greater leachate volume solid mass, larger proportion dissolves, increasing leaching efficiency.

Given constant total reactant mass, leachable quantity fixed.

Sufficient leachate maximizes concentration gradient, achieving theoretical maximum leaching efficiency Effect Concentration shown 5(a), comparison blank

experiment

added) demonstrates oxidation uranium tailings increases activity concentration solution approximately equilibrium. trend exhibits three sequential stages: rapid leaching, leaching, leaching equilibrium. identical leaching durations, higher concentrations

result

higher activity concentrations leaching rates solution, consistent leaching behavior uranium tailings primary cause observed variation Figure strong oxidizing action mechanism dissolves minerals, modifies surface chemistry minerals promote desorption (iii) elevates redox potential increase solubility Kurniawan thereby enhancing activity concentration solution.

Figure increase concentration proportional increases equilibrium concentration leaching rate. concentration rises, increases equilibrium concentration leaching initially increase subsequently decrease. behavior primarily attributed limited total amount oxidizable Pb-bearing minerals present tailings. concentrations, reaction predominantly controlled chemical reaction kinetics further increases concentration, dependence reaction concentration gradually diminishes (indicating reduction reaction order), readily reactive mineral phases progressively consumed, leaving reactive mineral phases.

Consequently, additional increases concentration, dissolution becomes difficult increase. leaching Concentration (mol/L) activity concentration function leaching different concentrations Leaching uranium tailings different concentrations Leaching behavior under different oxidation conditions Effect concentration curve Figure shows activity concentration increased sharply increase slowing system gradually approached equilibrium.

Concurrently, activity concentration exhibited significant fluctuations

throughout leaching process. behavior primarily attributed predominant adsorption mineral iron-manganese oxide surfaces through electrostatic forces. competitive cation, displacing adsorption sites facilitating rapid desorption weakly bound surfaces tailings particles Khalaji Khanday, Hamid During initial experimental phase, higher concentrations associated greater release, exchange predominated. later phase, strongly bound encapsulated within mineral lattice slowly released.

Subsequently, formed soluble complexes (e.g., (aq)), promoting dissolution solid phase.

However, concentrations, partial precipitation occurred.

Specifically, concentration exceeded mol/L, lead-containing complex solution partially precipitated inducing decline solution-phase concentration thereby generating significant fluctuations. stage, dissolution complexation inhibition precipitation collectively regulated process leaching leaching Variation 210Pb activity concentration leaching under different ionic strengths Variation cumulative activity concentration 210Pb solution function leaching Concentration (mol/L)

(c)Variation of 210Pb leaching rate from uranium tailings under different ionic strengths

Leaching behavior of 210Pb under different ionic strengths

elucidate effect varying concentrations activity concentrations Figure cumulatively summed, yielding trend depicted Figure curve demonstrates that, identical intervals, higher concentrations correlate increased cumulative activity concentrations solution, indicating elevated leaching rates

concentrations Figure corroborates observation, showing elevated concentrations

result

greater leaching rates These findings indicate stability

210 Pb

tailings highly dependent environmental ionic strength: under ionic strength conditions (e.g., rainwater, freshwater), firmly bound lower release risk, whereas under ionic strength conditions (e.g., seawater intrusion zones, saline-alkali soils, high-mineralization groundwater), desorption/dissolution significantly enhanced, leading substantial increase release Attallah Leaching Kinetics

Analysis

leaching radionuclides uranium tailings primarily involves sequential processes: diffusion radionuclides tailings surface, adsorption surface, surface reaction, desorption surface, diffusion products interface.

Consequently, diffusion, adsorption, chemical reaction, desorption collectively influence concentration solution. identify dominant mechanism under varying leaching conditions, fitted using pseudo-second-order kinetic model Chiron 2003; Baigenzhenov shrinking model 2010; two-constant model 2024; Jalali Avrami model Yazawa fitting curves presented Figure correlation coefficients summarized Tables Leaching time, Leaching time, Leaching time, Leaching time,

models

pH t / q t = a + k t 1-(1- α ) 1/3 =k t 1-(2/3) α -(1- α ) 2/3 = k t ln q t =a+k ∙ ln t -ln(1- α )=k t n

Based Table fitted curve, pseudo-second-order kinetic model provides indicating under varying conditions, leaching process governed chemical reaction solid surface rather diffusion process.

Consequently, reaction primarily determined chemical interaction reactants solid-liquid interface. conditions. coefficients determination Tables indicate leaching process controlled chemical reactions solid surface.

During experiment, depends factors including solid-to-liquid ratio concentration concentration overall reaction constant leaching expressed equation based Arrhenius equation Aghili where influence indices solid-to-liquid ratio concentration concentration respectively.

Taking natural logarithm sides equation yields equation Plots versus constructed, which following values obtained:

During experiment, temperature constant, leading equation where constant.

Thus, equation rewritten equation

Substituting equation pseudo-second-order kinetic model gives equation experimental substituted fitted x-axis y-axis, shown fitted data: =48.008 Therefore, leaching kinetic model given equation 4+48.008 Curve fitting

Analysis

Leaching Process Box-Behnken Design (BBD) employed optimize leaching process Mazurek-Ho independent variables solid-to-liquid ratio, concentration, concentration, leaching response. variable ranges consistent single-factor experiments: solid-to-liquid ratio concentration mol/L, concentration mol/L.

Experiments conducted sequentially according software-generated scheme,

results

presented Table Solid-to-liquid ratio

Analysis

variance significance tests performed established polynomial

model leaching rate, shown Table response surface model exhibited F-value 0.0001, indicating model leaching statistically significant overall effectively explains variation response variable. coefficient determination adjusted close demonstrating excellent model ability capture predominant patterns data. difference between adjusted confirming number independent variables matches sample size, thereby ensuring strong explanatory predictive power model experimental data.

Analysis

squares revealed factors influencing leaching rate, descending order influence, solid-to-liquid ratio, concentration, concentration. two-way interactions among factors significant, while quadratic terms, concentration significant, indicating nonlinear effect concentration. difference between experimental predicted leaching rates ranged +0.05, reflecting minimal prediction error.

Source Squares Square F-value p-value

Model 2.90 14 0.2074 50.81 < 0.0001

A-PH 0.2812 1 0.2812 68.90 < 0.0001

B-Solid-to-Liquid Ratio 1.87 1 1.87 458.15 < 0.0001

C-H ₂ O ₂ Concentration 0.4497 1 0.4497 110.18 < 0.0001

C ² 0.1728 1 0.1728 42.33 < 0.0001

R 2 =0.9807 R a dj 2 =0.9614 S/N=27.2907

Based leaching polynomial model, factors solid-to-liquid ratio, concentration, concentration selected independent variables, remaining factors midpoint values experimental design. response surface contour plots leaching shown Figures effects solid-to-liquid ratio leaching NaCl. solid-to-liquid ratio fixed 0.025, ranged leaching varied fixed solid-to-liquid ratio ranged leaching varied smaller variation range leaching versus solid-to-liquid ratio indicates

solid-to-liquid ratio exerts stronger influence leaching interaction experiment. smooth curvature contour lines suggests interaction effect between solid-to-liquid ratio leaching rate.

Figures effects concentration leaching solid-to-liquid ratio NaCl. concentration fixed ranged leaching varied fixed concentration ranged leaching exhibited distinct trend initial increase followed decrease, varying smaller variation range leaching versus concentration indicates exerts stronger influence leaching interaction experiment. pronounced curvature contour lines suggests strong interaction effect between concentration leaching Figures effects concentration leaching solid-to-liquid ratio concentration fixed ranged leaching exhibited pronounced curvature, varying fixed concentration ranged leaching varied larger variation range leaching versus concentration indicates exerts stronger influence leaching interaction experiment. smooth curvature contour lines suggests interaction effect between concentration leaching rate.

Figures effects solid-to-liquid ratio concentration leaching NaCl. concentration fixed solid-to-liquid ratio ranged leaching varied solid-to-liquid ratio fixed concentration ranged leaching varied 0.919, exhibiting pronounced curvature. larger variation range leaching solid-to-liquid ratio versus concentration indicates solid-to-liquid ratio exerts stronger influence leaching interaction experiment, leaching demonstrates nonlinear relationship concentration. smooth curvature contour lines suggests interaction effect between solid-to-liquid ratio concentration leaching rate.

Figures effects solid-to-liquid ratio concentration leaching concentration fixed solid-to-liquid ratio ranged leaching varied solid-to-liquid ratio fixed concentration ranged leaching varied larger variation range leaching solid-to-liquid ratio versus concentration indicates solid-to-liquid ratio exerts stronger influence leaching interaction experiment. straight-line pattern contour lines suggests significant interaction effect between solid-to-liquid ratio concentration leaching rate.

Figures effects concentration leaching solid-to-liquid ratio concentration fixed concentration ranged leaching varied 1.3368, exhibiting pronounced curvature. concentration fixed concentration ranged leaching varied

larger variation range leaching versus concentration indicates exerts stronger influence leaching interaction experiment. pronounced curvature contour lines suggests strong interaction effect between concentration leaching rate.

response surface contour Comparison contour curvature across reveals curvature magnitude decreases order indicating strong-to-weak interaction effect sequence concentration, concentration, solid-to-liquid ratio concentration, concentration solid-to-liquid ratio solid-to-liquid ratio concentration leaching rate.

Model optimization leaching maximized yielded optimal experimental conditions: solid-to-liquid ratio 0.025, concentration concentration achieving leaching

2.064%.

Conclusions

study, based self-made static leaching experimental setup, systematically investigated leaching behavior mechanism, leaching kinetics, interactive effects multiple environmental factors uranium tailings under static aqueous conditions.

conclusions

follows: Environmental factors exert decisive influence behavior mechanism leaching.

Under low-pH conditions (particularly leaching final concentration significantly enhanced through promotion mineral disintegration, increase specific surface reaction, competitive adsorption ions. solid-to-liquid ratio maintains concentration gradient diffusion driving force, facilitating greater contact between tailings leaching solution, thereby improving leaching efficiency. strong oxidizing property effectively promotes release disrupting crystal structure lead-bearing minerals altering mineral surface properties; however, enhancing effect exhibits nonlinear trend initial increase followed decrease concentration increases. primarily promotes leaching synergistically through exchange complexation concentrations (>0.3 mol/L), fluctuations leaching concentration arise precipitation.

Leaching kinetics

analysis

demonstrates throughout leaching process, leaching behavior described second-order kinetic model, primarily controlled chemical reaction solid-liquid interface rather diffusion.

Building model, empirical leaching kinetics model incorporating solid-to-liquid ratio, concentration, concentration parameters established, which effectively predicts leaching behavior under diverse environmental conditions. relative magnitudes effects various factors leaching their interaction effects determined. order influence leaching rate, greatest least, solid-to-liquid ratio concentration concentration.

Response surface

analysis

indicated strong interactive effects between concentration concentration, between concentration, while other factor interactions relatively weak.

Through model optimization, optimal parameters achieve maximum leaching (2.064%) determined solid-to-liquid ratio 0.025, concentration mol/L, concentration mol/L.

Declaration competing interest authors declare known competing financial interests personal relationships could appeared influence reported paper.

Acknowledgments

study financially supported Radiation Protection Laboratories (CIRPFSHJ2025004). authors appreciate comments anonymous reviewers improved quality manuscript

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