Migration of ammonium nitrogen in ion-absorbed rare earth soils during and post <i>in situ</i> mining: a column study and numerical simulation analysis

doi:10.1007/s11783-023-1702-4

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (8) : 102 https://doi.org/10.1007/s11783-023-1702-4

RESEARCH ARTICLE

Migration of ammonium nitrogen in ion-absorbed rare earth soils during and post in situ mining: a column study and numerical simulation analysis

Gaosheng Xi¹, Xiaojiang Gao^1,⁴(

), Ming Zhou¹, Xiangmei Zhai¹, Ming Chen², Xingxiang Wang³, Xiaoying Yang¹, Zezhen Pan^1,⁴(

), Zimeng Wang^1,^4,⁵

¹. Department of Environmental Science and Engineering, Fudan University, Shanghai 200438, China
². School of Resource and Environmental Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China
³. CAS Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China
⁴. National Observations and Research Station for Wetland Ecosystems of the Yangtze Estuary, Shanghai 202151, China
⁵. Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200001, China

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Abstract

● Column experiments with an inclined slope were applied to simulate NH₄–N transport.

● The transport of NH₄–N was simulated via HYDRUS-2D.

● The chemical non-equilibrium model well described the transport process.

● The lateral flow led to the preferential loss of surface NH₄–N.

● Flow rate and rainfall intensity affected the adsorption and leaching of NH₄–N.

Ion-absorbed rare earth mines, leached in situ, retain a large amount of ammonium nitrogen (NH₄–N) that continuously releases into the surrounding environments. However, quantitative descriptions and predictions of the transport of NH₄–N across mining area with hill slopes are not fully established. Here, laboratory column experiments were designed with an inclined slope (a sand box) to examine the spatial temporal transport of NH₄–N in soils collected from the ionic rare earth elements (REE) mining area. An HYDRUS-2D model simulation of the experimental data over time showed that soils had a strong adsorption capacity toward NH₄–N. Chemical non-equilibrium model (CNEM) could well simulate the transport of NH₄–N through the soil-packed columns. The simulation of the transport-adsorption processes at three flow rates of leaching agents revealed that low flow rate enabled a longer residence time and an increased NH₄-N adsorption, but reduced the extraction efficiency for REE. During the subsequent rainwater washing process, the presence of slope resulted in the leaching of NH₄–N on the surface of the slope, while the leaching of NH₄–N deep inside the column was inhibited. Furthermore, the high-intensity rainfall significantly increased the leaching, highlighting the importance of considering the impact of extreme weather conditions during the leaching process. Overall, our study advances the understanding of the transport of NH₄–N in mining area with hills, the impact of flow rates of leaching agents and precipitation intensities, and presents as a feasible modeling method to evaluate the environmental risks of NH₄–N pollution during and post REE in situ mining activities.

Keywords Ion-absorbed rare earth Ammonium nitrogen transport HYDRUS-2D Numerical simulation

Corresponding Author(s): Xiaojiang Gao,Zezhen Pan

Issue Date: 30 March 2023

Cite this article:

Gaosheng Xi,Xiaojiang Gao,Ming Zhou, et al. Migration of ammonium nitrogen in ion-absorbed rare earth soils during and post in situ mining: a column study and numerical simulation analysis[J]. Front. Environ. Sci. Eng., 2023, 17(8): 102.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1702-4
https://academic.hep.com.cn/fese/EN/Y2023/V17/I8/102

Tab.1 Physical properties of the collected soil sample

Fig.1 Experimental setup used for (a) water transport and prepared rainwater leaching; (b) ammonium nitrogen transport and chlorine tracer experiments. The labeled points in (a) represent the soil sample collection points and the holes in (b) represent soil solution collection points. The solution collection points at distances of 37.5, 32.5 27.5 and 22.5 cm were marked in (b).

$N H 4 +$ $(m g / L)$	$S O 4 2 −$ $(m g / L)$	$N O 3 −$ $(m g / L)$	$C l −$ $(m g / L)$	pH
0.13	1.32	0.74	0.24	5.85

Tab.2 Compositions of the artificial rainwater

Fig.2 Adsorption isotherms of ammonium nitrogen on ion-absorbed rare earths with model simulations of (a) Linear adsorption model; (b) Freundlich model; (c) Langmuir model, and desorption isotherms of ammonium nitrogen on ion-absorbed rare earths with model simulations of (d) Linear desorption model; (e) Freundlich model; (f) Langmuir model.

θ_r (cm³/cm³)	θ_s (cm³/cm³)	α (1/cm)	$n$	K_s (cm/h)	$l$
0.001	0.5612	0.0049	1.6826	1.1513	0.5

Tab.3 Hydraulic parameters in the HYDRUS-2D model

Fig.3 Observed and simulated water content of water transport experiments at a temperature of 20.0 ± 0.2 °C at a flow rate of 15 mL/min, measured at conditions of (a) 0 h after the end of water transport; (b) 24 h after the end of water transport.

Fig.4 Observed and simulated breakthrough curves of the conservative tracer (Cl⁻) experiment measured at the position of (a) (5.0 cm, 15.0 cm), (5.0 cm, 52.5 cm) and (5.0 cm, 90.0 cm); (b) (25.0 cm, 15.0 cm), (25.0 cm, 47.5 cm) and (25.0 cm, 80.0 cm); (c) (45.0 cm, 15.0 cm), (45.0 cm, 42.5 cm) and (45.0 cm, 70.0 cm); (d) (65.0 cm, 15.0 cm), (65.0 cm, 37.5 cm) and (65.0 cm, 60.0 cm). (Cl⁻ concentration = 0.76 g/L; t = 20.0 ± 0.2 °C; flow rate = 15 mL/min).

Fig.5 Observed and simulated breakthrough curves of ammonium ions transport experiments at a temperature of 20.0 ± 0.2°C at a flow rate of 15 mL/min, measured at the position of (a) (5.0 cm, 90.0 cm); (b) (5.0 cm, 52.5 cm); (c) (5.0 cm, 15.0 cm); (d) (25.0 cm, 80.0 cm); (e) (25.0 cm, 47.5 cm); (f) (25.0 cm, 15.0 cm); (g) (45.0 cm, 70.0 cm); (h) (45.0 cm, 42.5 cm); (i) (45.0 cm, 15.0 cm); (j) (65.0 cm, 60.0 cm); (k) (65.0 cm, 37.5 cm); (l) (65.0 cm, 15.0 cm). CNEM represents the chemical non-equilibrium model.

	$K d$ $(L / k g)$	$ω$ $(1 / h)$	f	MAE $(m g / L)$	RMSE $(m g / L)$	r
CDEM	1.185	0	1	18.83	45.64	0.927
One-site CNEM	1.538	0.451	0	9.09	20.68	0.983
Two-site CNEM	1.690	8.892	0.226	6.21	13.89	0.993

Tab.4 Solute transport parameters for ammonium nitrogen transport-adsorption in the HYDRUS-2D model and parameter evaluation

	$K d$ $(L / k g)$	$ω$ $(1 / h)$	f	MAE $(m g / L)$	RMSE $(m g / L)$	r
CDEM	0.950	0	1	68.86	84.13	0.771
One-site CNEM	1.680	0.625	0	18.07	22.31	0.979
Two-site CNEM	1.661	0.625	0.064	24.37	26.90	0.977

Tab.5 Solute transport parameters for ammonium nitrogen leaching in the HYDRUS-2D model and parameter evaluation

Fig.6 Simulated soil ammonium nitrogen pollution patterns in the profile after 96 h in the ammonium nitrogen leaching experiment by (a) equilibrium model; (b) one-site CNEM; (c) two-site CNEM; (d) correlation between measured and simulated soil ammonium nitrogen concentration by equilibrium model, one-site CNEM and two-site CNEM at a temperature of 20.0 ± 0.2°C at the precipitation of 10 mm/h.

Fig.7 Temporal variation of ammonium nitrogen transport-adsorption amount in column experiment (ammonium nitrogen concentration = 0.30 g/L; t = 20.0 ± 0.2 °C; flow rate = 15 mL/min). The labeled values on the right of the figure were the adsorbed amounts of ammonium nitrogen by the soil within every 60 h. For instance, the value of 9.49 g was the adsorbed amount of ammonium nitrogen by the soil from 120th to 180th h.

Fig.8 Variation of ammonium nitrogen pollution patterns in the simulated profile during ammonium nitrogen leaching at the time of (a) 24th hour; (b) 48th hour; (c) 72nd hour; (d) distribution of ammonium nitrogen concentration with depth in the middle of the simulated profile at the 24th hour, the 48th hour and the 72nd hour at the precipitation of 10 mm/h.

Fig.9 Variation of ammonium nitrogen pollution patterns in the simulated profile during ammonium nitrogen transport-adsorbing at a flow rate of (a) 5 mL/min; (b) 10 mL/min; (c) 15 mL/min; (d) cumulative loss flux of ammonium nitrogen during transport-adsorbing at flow rates of 5 , 10 and 15 mL/min, total time as 432 h.

Fig.10 Variation of ammonium nitrogen pollution patterns in the simulated profile during ammonium nitrogen leaching at the precipitation of (a) 4 cm/d; (b) 8 cm/d; (c) 12 cm/d; (d) cumulative leaching flux of ammonium nitrogen during ammonium nitrogen leaching at the precipitations of 4 , 8 and 12 cm/d, total time as 432 h.

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