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Chloroquine degradation in aqueous solution under electron beam irradiation

Stephen Kabasa
Stephen Kabasa
, 
Yongxia Sun
Yongxia Sun
, 
Sylwester Bułka
Sylwester Bułka
 und 
Andrzej G. Chmielewski
Andrzej G. Chmielewski
   | 25. Juni 2024
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Article Category: Original Paper
Online veröffentlicht: 25. Juni 2024
Seitenbereich: 53 - 63
Eingereicht: 05. Okt. 2023
Akzeptiert: 16. Feb. 2024
DOI: https://doi.org/10.2478/nuka-2024-0008
Schlüsselwörter
© 2024 Stephen Kabasa et al., published by Sciendo
This work is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

Fig. 1.

UV-VIS absorption spectrum for 125 mg·L 1 chloroquine solution observed at 343 nm at irradiation doses ranging from 0 kGy to 7 kGy.
UV-VIS absorption spectrum for 125 mg·L 1 chloroquine solution observed at 343 nm at irradiation doses ranging from 0 kGy to 7 kGy.

Fig. 2.

Degradation of 125 mg·L-1 of chloroquine solution under EB radiation.
Degradation of 125 mg·L-1 of chloroquine solution under EB radiation.

Fig. 3.

Degradation of different concentrations of chloroquine solutions under EB irradiation. (a) Removal efficiency of chloroquine at different initial concentrations. (b) k (kGy-1) values for removal of chloroquine at 0.5 kGy. (c) Plot of the rate constant against dose.
Degradation of different concentrations of chloroquine solutions under EB irradiation. (a) Removal efficiency of chloroquine at different initial concentrations. (b) k (kGy-1) values for removal of chloroquine at 0.5 kGy. (c) Plot of the rate constant against dose.

Fig. 4.

Removal efficiency of 125 mg·L 1 of chloroquine solution under EB irradiation at different initial pH.
Removal efficiency of 125 mg·L 1 of chloroquine solution under EB irradiation at different initial pH.

Fig. 5.

Changes in the pH of the solution with dose during the degradation of 125 mg·L-1 chloroquine solution.
Changes in the pH of the solution with dose during the degradation of 125 mg·L-1 chloroquine solution.

Fig. 6.

Changes in the pH concentration during EB irradiation of 125 mg·L-1 chloroquine. The pH varied from slightly acidic before irradiation to acidic at the end of irradiation.
Changes in the pH concentration during EB irradiation of 125 mg·L-1 chloroquine. The pH varied from slightly acidic before irradiation to acidic at the end of irradiation.

Fig. 7.

Release of Cl with increasing dose during radiolysis of chloroquine (125 mg·L-1) solution under the EB treatment.
Release of Cl with increasing dose during radiolysis of chloroquine (125 mg·L-1) solution under the EB treatment.

Fig. 8.

(a) Reduction in total Kjeldahl nitrogen, formation of NO3−, and (b) generation of NH4+ in the degradation of 125 mg·L-1 of chloroquine solution under EB irradiation.
(a) Reduction in total Kjeldahl nitrogen, formation of NO3−, and (b) generation of NH4+ in the degradation of 125 mg·L-1 of chloroquine solution under EB irradiation.

Fig. 9.

Changes in dissolved oxygen concentration during electron beam irradiation of 125 mg·L-1 chloroquine solution.
Changes in dissolved oxygen concentration during electron beam irradiation of 125 mg·L-1 chloroquine solution.

Fig. 10.

Variation in COD and TOC during EB degradation of 125 mg·L-1 solution of chloroquine.
Variation in COD and TOC during EB degradation of 125 mg·L-1 solution of chloroquine.

Species formed in the radiolysis of water and their corresponding G-values and reaction rates (k) with CQ

Species G (mmol·J-1) Molecules/100 eV k (dm3·mol-1·s-1)
eaq− 0.28 2.8 4.8 × 1010
•OH 0.28 2.8 7.3 × 109
•H 0.06 0.6 –
H3O+ 0.26 2.6 –
H2 0.045 0.45
H2O2 0.07 0.7

Methods previously used for the removal of CQ from aqueous solutions

Methods Conditions Removal efficiency Ref.
Membranes
Membrane bioreactors – tyrosinase enzyme on Escherichia coli biopolymer pH 7.5, 20 h 98% with 140 ± 6 mg·g-1 No apparent capacity loss over three consecutive cycles [33]
Adsorbents
Activated carbon Palm kernel (Elaeis guineensis) shells Large surface areas, strong mechanical characteristics [27]
PPAC-ZnO 313 K 10 ppm CQ 78.89% Adsorption capacity increases with temperature [28]
A-GO hydrogel Adsorption 63 mg·g-1 [29, 30]
GAC-GO Equilibrium time 18 h 37.65 mg·g-1 Adsorption [32]
Organo-clay raw kaolinite treated with citric acid 20 mg·L-1 CQ 120 min 99.28% Maximum sorption capacity is 4.03 mg·g-1
Soybean hull residues functionalized with iron oxide nanoparticles (SBH-Fe3O4) 120 min 318 K Adsorption capacity 98.84 mg·g-1 Reuse five cycles [34]
Iron and magnesium comodified rape straw biochar (Fe/Mg-RSB) pH (3–11) CQ 4–25 mg·L-1 at 180 r·min-1 for 8 h 308 K Adsorption capacity of 42.93 mg·g-1 [35]
MOF sheet, namely BUC-21(Fe) FeSO4·7H2O, 1,3-dibenzyl-2-imidazoli-done-4,5-dicarboxylic acid (H2L) and 4,4’-bipyridine (bpy) pH = 5.0 30 min 100% C•OH 242.5 mmol·L-1, H2O2 consumption 83.2% [36]
Catalysts
Ferrate-Fe(VI) CQ 10 μM Fe(VI) 40–180 mM time 1–20 min 59% CQ removal Algae, antimicrobial, toxicity reduction [19]
CWAO HEO – (MgCuMnCoFe) Ox Oxygen pressure of 15 bar, catalyst dosage of 1.4 g·L-1, and temperature of 230°C 34.6% and 41.2% higher than that without the HEO system [11]
Single cobalt atoms in a defined Co–N3 coordination structure pH range (3–11) employing the SA Co-N-C (30) 100% [24, 25]
Biochar-supported RM-BC activated persulfate process 20 mg·L-1 40 min 84.8% [26]
Carbon nanotube-loaded CoFe2O4 (CoFe2O4@CNTs) composite 10 mg·L-1 CQ pH 7 Mineralization efficiency 33%, removal efficiency 98.7% [37]
Advanced oxidation processes
SR-AOP Peroxymonosulfate (PMS, HSO5−) peroxy disulfate (PDS, S2O82−) 10.0 mg·L-1 P25M175-94.6% within 30 min [23]
UV/PS pH = 6.9 10 min 91.3% CQ reactions with •OH and SO4·− were 8.9 × 109 L·(mol·s)-1 and 1.4 × 1010 L·(mol·s)-1 [38]
Photocatalysis-activated SR-AOP over PDINH/MIL-88A(Fe) composites 10.0 mg·L-1 CQ P25M175 30 min 94.6% Good reusability and stability [23]
Electrocoagulation 66.89 mA·cm–2, 600 rpm 60 min electrolysis time 3 mg·L-1 CQ, pH = 6.5 95% dissolved aluminum electrodes 0.228 kg·m-3 energy consumption of 12.243 kWh·m-3 [39]
EFP Carbon felt cathode and BDD anode 92% (TOC) [20]
FBER BDD electrodes batch recirculation mode 9 h, pH 5.38, 34.4 mA·cm-2, and liquid flow rate (Q) of 1.42 L·min-1 Degradation 89.3%, COD 51.6%, mineralization 53.1% energy consumption 0.041 kWh·L-1 [40]
Electro-Fenton with pyrite (FeS2)-modified graphite felt (FeS2/GF) cathode pH of 3.0 FeS2 loading-10 mg, current density 150 mA, electrode spacing 2.0 cm 83.3 ± 0.4% 60 min CQ removal, retains 60.0% CQ removal in consecutive batch tests [41]

Reaction rates (k) for degradation of different concentrations of chloroquine and corresponding R2

Concentration CQ (mg·L-1) k (kGy-1) R2
 75 1.6567 0.9935
100 1.3603 0.9982
125 1.1224 0.9891
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