Obiri-Nyarko F; Darko DA; Quansah JO; Asare SV; Karikari AY

doi:10.26599/JGSE.2025.9280060

doi: 10.26599/JGSE.2025.9280060

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出版历程
- 收稿日期: 2024-09-25
- 录用日期: 2025-08-21
- 网络出版日期: 2025-10-10
- 刊出日期: 2025-12-01

Natural brown coal as an adsorbent for manganese removal from groundwater: A mechanistic and operational evaluation

1.
Groundwater and Geoscience Division, CSIR-Water Research Institute, P.O. Box M32, Accra, Ghana
2.
Institute for Environment and Sanitation Studies, College of Basic and Applied Sciences, University of Ghana, Legon, Accra – Ghana
3.
Environmental Chemistry and Sanitation Engineering Division, CSIR-Water Research Institute, P.O. Box M32, Accra, Ghana

More Information

Corresponding author: Fobiri-nyarko@csir.org.gh

摘要

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Abstract: This study investigates the potential of natural Brown Coal (BC) as a sustainable, cost-effective adsorbent for the removal of manganese (Mn²⁺) from contaminated groundwater. A series of batch adsorption experiments was conducted to assess the influence of key operational parameters—such as solution pH, initial Mn²⁺ concentration, BC dosage, temperature, and the presence of competing ions—on Mn²⁺ removal efficiency. The environmental compatibility and regeneration potential of BC were also evaluated to determine its practical viability for repeated use. To better understand the adsorption behaviour, equilibrium and kinetic data were analysed using established isotherm and kinetic models, while thermodynamic parameters were computed to assess the spontaneity and thermal characteristics of the adsorption process. Furthermore, geochemical modelling and comprehensive BC characterization—including surface morphology, mineralogical and elemental composition, and functional group analysis—were performed to elucidate Mn²⁺ speciation under varying environmental conditions and to uncover the underlying adsorption mechanisms. Results showed that Mn²⁺ removal efficiency increased with higher pH, temperature, and BC dosage, but declined at elevated initial Mn²⁺ concentrations due to active site saturation. The process was spontaneous and endothermic, with the Langmuir isotherm model (R² = 0.994) and pseudo-second-order kinetic model (R² = 0.996) providing the best fit to experimental data. Mechanistic analysis indicated that chemisorption, primarily through ion exchange and inner-sphere complexation, was the dominant mode of Mn²⁺ uptake. The presence of competing cations, especially Fe³⁺ and Cu²⁺, significantly hindered Mn²⁺ removal due to preferential binding. Importantly, BC exhibited strong reusability, maintaining over 80% removal efficiency across four adsorption–desorption cycles without evidence of secondary pollutants. These findings demonstrate the potential of natural BC as an efficient, reusable, and environmentally benign material for treating manganese-contaminated groundwater.
- Sorption /
- Surface complexation /
- Ion exchange /
- Geochemical modelling /
- Heavy metals /
- Secondary pollution

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Figure 1. Characterization results showing: (a) Point of zero charge, (b) X-ray diffraction spectrum, (c) SEM, and (d) EDX images of the unloaded BC

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Figure 2. Effect of initial solution pH on Mn²⁺ removal by BC

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Figure 3. The impact of (a) BC dosage and (b) initial Mn²⁺ concentration on Mn²⁺ adsorption

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Figure 4. Effect of coexisting ions (Na⁺, K⁺, Ca²⁺, Cu²⁺, Zn²⁺, Fe³⁺ at concentrations of 5 mg/L, 10 mg/L, and 15 mg/L) on Mn²⁺ adsorption by BC

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Figure 5. Mn²⁺ experimental data fitted with (a) Freundlich and (b) Langmuir isotherms

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Figure 6. Evaluation of Mn²⁺ adsorption kinetic data with (a) pseudo-first-order and pseudo-second-order models and (b) the intra-particle diffusion model

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Figure 7. Results of experiments to study (a) the reusability of the BC, and (b) the environmental benignity of the BC (Adsorbent mass: 1 g; pH = 6)

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Figure 8. (a) Net concentrations of Ca²⁺, Na⁺, Mg²⁺, K⁺ and Mn²⁺ eluted/adsorbed into solution at different solution pH values, and (b) FTIR spectra of the BC before and after loading with Mn²⁺

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Table 1. Basic summary characteristics of the BC

Parameters	Value
pH_pzc	4.02
Moisture (%)	5.30
Ash content (%)	7.90
Volatile matter (%)	30.10
Fixed carbon (%)	56.70
Pore volume (cm³/g)	0.017
Surface area (m²/g)	6.70
Elemental composition (%)
Carbon	65.68
Oxygen	24.61
Ca	2.00
Si	3.01
Al	2.37

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Table 2. Thermodynamic parameters for Mn²⁺ adsorption on BC

Temperature K	∆G^○ kJ/mol	∆H^○ kJ/mol	∆S^○ kJ/mol-K
298	−4.89	15.53	0.069
323	−6.73
348	−8.42
363	−9.12
373	−10.08
393	−11.55

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Table 3. Comparison of Mn²⁺ adsorption capacity (Q_max) obtained in this study with those reported for other natural and low-cost adsorbents in previous studies

Adsorbent	Q_max/mg/g	Particle size	pH	Temperature/°C	Reference
Zeolite Y	0.015	0.75 µm	6.50	25	Kwakye-Awuah et al. 2019
Phoenix dactylifera L. seed	0.361	NA	7.0	NA	Osundiya et al. 2024
Date palm biochar	0.44	0.15 mm	6	NA	Fseha et al. 2022
Tea waste	0.158	2 mm	NA	NA	Badrealam et al. 2019
BC	1.190	75 µm	6.00	25	This study
Q_max: Maximum adsorption capacity; NA = not available

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Table 4. Parameters of the PFK, PSK and IPD models

PFK			PSK			IPD
q_e (mg/g)	k₁ (1/h)	R²	q_e (mg/g)	k₂ (mg/g h)	R²	k_p1 (mg/g min^1/2)	R²	k_p2 (mg/g min^1/2)	R²
0.259	0.070	0.988	0.268	0.673	0.996	0.005	0.913	0.0008	0.722

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Table 5. Physico-chemical properties of real groundwater before and after BC treatment

Parameter	Unit	Before BC	After BC	WHO (2017)
Turbidity	NTU	59.2	2.09	5
Colour (apparent)	Hz	75.0	5.00	5
pH	pH Units	6.21	6.57	6.5–8.5
Conductivity	µS/cm	531	623	-
TSS	mg/l	49.0	1.00	-
TDS	mg/l	293	343	1,000
Sodium	mg/l	16.0	56.0	200
Potassium	mg/l	6.00	3.30	30
Calcium	mg/l	24.0	28.9	200
Magnesium	mg/l	21.7	20.7	150
Total Iron	mg/l	18.0	0.401	0.3
Ammonium (NH₄-N)	mg/l	0.001	<0.001	0.00–1.5
Chloride	mg/l	76.9	185	250
Sulphate (SO₄)	mg/l	18.7	16.10	250
Manganese	mg/l	10.20	1.14	0.4
Nitrite (NO₂-N)	mg/l	0.036	<0.001	1
Nitrate (NO₃-N)	mg/l	0.111	0.247	10
Total Hardness (as CaCO₃)	mg/l	150	157	500
Bicarbonate (as CaCO₃)	mg/l	77.6	14.4	-

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