Study of diclofenac removal by the application of combined zero-valent iron and calcium peroxide nanoparticles in groundwater

Liang Wen; Zhou Nian-qing; Dai Chao-meng; Duan Yan-ping; Zhou Lang; Tu Yao-jen

doi:10.19637/j.cnki.2305-7068.2021.03.001

2021 Vol. 9, No. 3

Article Contents

Article navigation > Journal of Groundwater Science and Engineering > 2021 > 9(3): 171-180

Next Article Previous Article

Liang Wen, Zhou Nian-qing, Dai Chao-meng, Duan Yan-ping, Zhou Lang, Tu Yao-jen. 2021. Study of diclofenac removal by the application of combined zero-valent iron and calcium peroxide nanoparticles in groundwater. Journal of Groundwater Science and Engineering, 9(3): 171-180. doi: 10.19637/j.cnki.2305-7068.2021.03.001

Citation:

Liang Wen, Zhou Nian-qing, Dai Chao-meng, Duan Yan-ping, Zhou Lang, Tu Yao-jen. 2021. Study of diclofenac removal by the application of combined zero-valent iron and calcium peroxide nanoparticles in groundwater. Journal of Groundwater Science and Engineering, 9(3): 171-180. doi: 10.19637/j.cnki.2305-7068.2021.03.001

Study of diclofenac removal by the application of combined zero-valent iron and calcium peroxide nanoparticles in groundwater

1.
College of Civil Engineering, Tongji University, Shanghai 200092, China
2.
School of Environmental and Geographical Sciences, Shanghai Normal University, Shanghai 200234, China
3.
Department of Civil, Architectural and Environmental Engineering, University of Texas at Austin, USA

More Information

Corresponding author: nq.zhou@tongji.edu.cn

Received Date: 20 May 2021

Accepted Date: 25 July 2021

Publish Date: 15 September 2021

Abstract

Abstract

Diclofenac (DCF) is one of the most frequently detected pharmaceuticals in groundwater, posing a great threat to the environment and human health due to its toxicity. To mitigate the DCF contamination, experiments on DCF degradation by the combined process of zero-valent iron nanoparticles (nZVI) and nano calcium peroxide (nCaO₂) were performed. A batch experiment was conducted to examine the influence of the adding dosages of both nZVI and nCaO₂ nanoparticles and pH value on the DCF removal. In the meantime, the continuous-flow experiment was done to explore the sustainability of the DCF degradation by jointly adding nZVI/nCaO₂ nanoparticles in the reaction system. The results show that the nZVI/nCaO₂ can effectively remove the DCF in the batch test with only 0.05 g/L nZVI and 0.2 g/L nCaO₂ added, resulting in a removal rate of greater than 90% in a 2-hour reaction with an initial pH of 5. The degradation rate of DCF was positively correlated with the dosage of nCaO₂, and negatively correlated with both nZVI dosage and the initial pH value. The order of significance of the three factors is identified as pH value > nZVI dosage > nCaO₂ dosage. In the continuous-flow reaction system, the DCF removal rates remained above 75% within 150 minutes at the pH of 5, with the applied dosages of 0.5 g/L for nZVI and 1.0 g/L for nCaO₂. These results provide a theoretical basis for the nZVI/nCaO₂ application to remove DCF in groundwater.
- Nanoscale zero-valent iron (nZVI) /
- Nano calcium peroxide (nCaO₂) /
- Diclofenac /
- Fenton-like reaction /
- Groundwater pollution

FullText(HTML)

References

[1]	Abraham N, Daniel C. 2008. Calcium peroxide (CaO₂) for use in modified Fenton chemistry. Journal of Hazardous Materials, 152(3): 1164-1170. doi: 10.1016/j.jhazmat.2007.07.096 CrossRef Google Scholar
[2]	Bin W, Shu-bo D, Jun H, et al. 2013. Environmental risk assessment and control of emerging contaminants in China. Environmental Chemistry(7): 1129-1136. doi: 10.7524/j.issn.0254-6108.2013.07.003 CrossRef Google Scholar
[3]	Einsiedl F, Radke M, Maloszewski P. 2010. Occurrence and transport of pharmaceuticals in a karst groundwater system affected by domestic wastewater treatment plants. Journal of Contaminant Hydrology, 117(1): 26-36. doi: 10.1016/j.jconhyd.2010.05.008 CrossRef Google Scholar
[4]	Forrez I, Carballa M, Verbeken K, et al. 2010. Diclofenac oxidation by biogenic manganese oxides. Environmental Science and Technology, 44(9): 3449-3454. doi: 10.1021/es9027327 CrossRef Google Scholar
[5]	Gomes DS, Gando-Ferreira LM, Quinta-Ferreira RM, et al. 2018. Removal of sulfamethoxazole and diclofenac from water: Strategies involving O₃ and H₂O₂. Environmental Technology, 39(13): 1658-1669. doi: 10.1080/09593330.2017.1335351 CrossRef Google Scholar
[6]	Joo SH, FEITZ AJ, WAITE TD. 2004. Oxidative degradation of the carbothioate herbicide, molinate, using nanosoale zero-valent iron. Environmental Science and Technology, 38(7): 2242-2247. doi: 10.1021/es035157g CrossRef Google Scholar
[7]	Jurado A, Walther M, Díaz-Cruz MS. 2019. Occurrence, fate and environmental risk assessment of the organic microcontaminants included in the Watch Lists set by EU Decisions 2015/495 and 2018/840 in the groundwater of Spain. Science of the Total Environment, 663: 285-296. doi: 10.1016/j.scitotenv.2019.01.270 CrossRef Google Scholar
[8]	Li R, Jin X, Megharaj M, et al. 2015. Heterogeneous Fenton oxidation of 2,4-dichlorophenol using iron-based nanoparticles and persulfate system. Chemical Engineering Journal, 264: 587-594. doi: 10.1016/j.cej.2014.11.128 CrossRef Google Scholar
[9]	Liang W, Dai CM, Zhou XF, et al. 2014. Application of zero-valent iron nanoparticles for the removal of aqueous zinc ions under various experimental conditions. Plos One, 9(1): e85686. doi: 10.1371/journal.pone.0085686 CrossRef Google Scholar
[10]	Liang W, Zhou NQ, Dai C M, et al. 2020. Zero-valent iron nanoparticles and its combined process for diclofenac degradation under various experimental conditions. Polish Journal of Environmental Studies, 30(2): 1279-1288. doi: 10.15244/pjoes/123921 CrossRef Google Scholar
[11]	Mikhailov I, Komarov S, Levina V, et al. 2017. Nanosized zero-valent iron as Fenton-like reagent for ultrasonic-assisted leaching of zinc from blast furnace sludge. Journal of Hazardous Materials, 321: 557-565. doi: 10.1016/j.jhazmat.2016.09.046 CrossRef Google Scholar
[12]	Muhammad U, Hamidi Abdul A, Mohd Suffian Y. 2010. Trends in the use of Fenton, electro-Fenton and photo-Fenton for the treatment of landfill leachate. Waste Management, 30(11): 2113-2121. doi: 10.1016/j.wasman.2010.07.003 CrossRef Google Scholar
[13]	Mutiyar PK, Gupta SK, Mittal AK. 2018. Fate of pharmaceutical active compounds (PhACs) from River Yamuna, India: An ecotoxicological risk assessment approach. Ecotoxicology and Environmental Safety, 150(15): 297-304. doi: 10.1016/j.ecoenv.2017.12.041 CrossRef Google Scholar
[14]	Qian Y, Zhou X, Zhang Y, et al. 2013. Performance and properties of nanoscale calcium peroxide for toluene removal. Chemosphere, 91(5): 717-723. doi: 10.1016/j.chemosphere.2013.01.049 CrossRef Google Scholar
[15]	Schwaiger J, Ferling H, Mallow U, et al. 2004. Toxic effects of the non-steroidal anti-inflammatory drug diclofenac: Part I: Histopathological alterations and bioaccumulation in rainbow trout. Aquatic Toxicology, 68(2): 141-150. doi: 10.1016/j.aquatox.2004.03.014 CrossRef Google Scholar
[16]	Shen J, Ou C, Zhou Z, et al. 2013. Pretreatment of 2,4-dinitroanisole (DNAN) producing wastewater using a combined zero-valent iron (ZVI) reduction and Fenton oxidation process. Journal of Hazardous Materials, 260: 993-1000. doi: 10.1016/j.jhazmat.2013.07.003 CrossRef Google Scholar
[17]	Shirazi E, Torabian A, Nabi Bidhendi G. 2013. Carbamazepine removal from groundwater: Effectiveness of the TiO₂/UV, nanoparticulate zero-valent iron, and Fenton (nZVI/H₂O₂) processes. Clean - Soil Air Water, 41(11): 1062-1072. doi: 10.1002/clen.201200222 CrossRef Google Scholar
[18]	Singh R, Misra V, Mudiam MKR, et al. 2012. Degradation of γ-HCH spiked soil using stabilized Pd/Fe⁰ bimetallic nanoparticles: Pathways, kinetics and effect of reaction condition. Journal of Hazardous Materials, 237-238: 355-364. doi: 10.1016/j.jhazmat.2012.08.064 CrossRef Google Scholar
[19]	Stefaniuk M, Oleszczuk P, Ok YS. 2016. Review on nano zerovalent iron (nZVI): From synthesis to environmental applications. Chemical Engineering Journal, 287: 618-632. doi: 10.1016/j.cej.2015.11.046 CrossRef Google Scholar
[20]	Sun YP, Li XQ, Cao J, et al. 2006. Characterization of zero-valent iron nanoparticles. Advances in Colloid and Interface Science, 120(1-3): 47-56. doi: 10.1016/j.cis.2006.03.001 CrossRef Google Scholar
[21]	Vieno N, Sillanpää M. 2014. Fate of diclofenac in municipal wastewater treatment plant – A review. Environment International, 69: 28-39. doi: 10.1016/j.envint.2014.03.021 CrossRef Google Scholar
[22]	Vilardi G, Sebastiani D, Miliziano S, et al. 2018. Heterogeneous nZVI-induced Fenton oxidation process to enhance biodegradability of excavation by-products. Chemical Engineering Journal, 335: 309-320. doi: 10.1016/j.cej.2017.10.152 CrossRef Google Scholar
[23]	Vymazal J, Dvořáková Březinová T, Koželuh M, et al. 2017. Occurrence and removal of pharmaceuticals in four full-scale constructed wetlands in the Czech Republic–the first year of monitoring. Ecological Engineering, 98: 354-364. doi: 10.1016/j.ecoleng.2016.08.010 CrossRef Google Scholar
[24]	Wang HF, Zhao YS, Li TY, et al. 2016. Properties of calcium peroxide for release of hydrogen peroxide and oxygen: A kinetics study. Chemical Engineering Journal, 303: 450-457. doi: 10.1016/j.cej.2016.05.123 CrossRef Google Scholar
[25]	Zhang W, Gao H, He J, et al. 2017. Removal of norfloxacin using coupled synthesized nanoscale zero-valent iron (nZVI) with H₂O₂ system: Optimization of operating conditions and degradation pathway. Separation and Purification Technology, 172: 158-167. doi: 10.1016/j.seppur.2016.08.008 CrossRef Google Scholar