Elsevier

Chemosphere

Volume 286, Part 2, January 2022, 131722
Chemosphere

Comparative study on the removal of organic pollutants by magnetic composite and pre-magnetized zero-valent iron activated persulfate

https://doi.org/10.1016/j.chemosphere.2021.131722Get rights and content

Highlights

  • Waste cartons derived magnetic composite was fabricated from hydrothermal conversion.

  • The composite could be served as an efficient activator of PS and be recycled multiple times.

  • Magnetic memory decay over time in the Pre-ZVI/PS treatment process was revealed.

  • Lignocellulosic biomass derived carbon is worth exploiting as activators for the actual application.

Abstract

The rapid development of global logistics has led to the overuse of packaging cartons, causing problems for municipal solid waste disposal. Diverse methods of exploiting the potential value of waste cartons are needed. Herein, we fabricated a magnetic composite (MC) from waste cartons via a one-step hydrothermal treatment and characterized. Using methylene blue (MB) as a model organic pollutant, tests of the activation of persulfate (PS) via the MC for the removal of MB were performed. Meanwhile, a comparison with activation with pre-magnetized zero-valent iron (Pre-ZVI/PS) was made. The comparative results show that the removal of MB was successfully accomplished with both Pre-ZVI/PS and MC/PS. Specifically, MC/PS could remove almost 100 % of MB, with the COD removal efficiency reaching over 70 % when the MB concentration was 50 mg/L at 80 min under different pH conditions. Even when reused twice, the MC still displayed robust activation performance. Additionally, we evaluated the lifetime of magnetic memory for Pre-ZVI, and first found its consecutive loss of pre-magnetization over 30 days, corresponding to the incremental attenuation of reaction rate constants in the Pre-ZVI-activated PS process. Overall, activating PS using the MC is a promising advanced oxidation technology and also provides a valuable reference on the valorization of lignocellulosic biomass.

Introduction

Over the past few years, a series of reports have demonstrated the enhanced removal of heavy metals or organic pollutants via zero-valent iron (ZVI) coupled with a weak magnetic field (WMF) (Wu et al., 2018, 2020a). As extension of this research “boom”, using pre-magnetized ZVI (Pre-ZVI) to activate persulfate (PS) for organic pollutant removal has been drawing increasing attention, because the performance of Pre-ZVI is superior to that of pristine ZVI (Li et al., 2015; Pan et al., 2018; Xu et al., 2016; Zhang et al., 2019). However, the lifetime of the “magnetic memory” of Pre-ZVI (under the influence of the earth's magnetic field) is critical to practical applications. While a handful of studies explored the effects of different pre-magnetization methods on the removal of target pollutants, long-term observations of the lifetime of magnetic memory were scarcely reported (Huang et al., 2018; Pan et al., 2018; Wu et al., 2020a).

In addition to the activation of PS via ZVI (including using Pre-ZVI), attempts to activate PS using carbon-bearing materials continue to be reported, suggesting that this is also a viable activation method (Cheng et al., 2019; Dong et al., 2019; Zhang et al., 2021). Waste carbon-bearing stuff is ubiquitous in the environment, and it will be of great environmental significance if we can make full use of it for PS activation. Lignocellulose is a sustainable alternative to diminishing fossil resources and the most abundant renewable biomass resources in natural environment (Guan et al., 2020). Over the past decades, online shopping has become a popular lifestyle, accompanied by the rapid development of the logistics industry. Due to the extensive use of packaging carton worldwide (Clomburg et al., 2017; Wang et al., 2020), massive quantities of them are discarded in urban areas every day, causing an increasing burden for municipal solid waste (MSW) disposal. Our previous study successfully fabricated C/Fe composites via a three-step process from waste cartons; the composites exhibited good adsorption of selected dyes (Wu et al., 2020b). The present study seeks to discover whether these types of composites prepared from waste cartons can be efficiently applied to activate PS, and to compare their performance with that of Pre-ZVI activated PS (Pre-ZVI/PS).

In this study, considering the potential value of waste cartons and the previous fabrication process, we attempted to prepare MC via a one-step hydrothermal process from waste cartons for valorization, and to use that composite to activate PS (MC/PS) for treating organic pollutants. The objectives of this research are to (i) compare the removal efficiencies of MB for both MC/PS and Pre-ZVI/PS; (ii) scrutinize the property of the MC to further unravel the internal reaction mechanism; (iii) identify the transformation products of MB by liquid chromatography tandem mass spectrometry (LC-MS/MS). The novelty lies in MB removal by MC/PS from waste cartons and the findings of magnetic memory decay over 30 days in the Pre-ZVI/PS treatment. This study aims to propose a new environmentally friendly and low-cost advanced oxidation process (AOP) for wastewater treatment, which could be adopted for the highly efficient removal of organic pollutants.

Section snippets

Chemicals

Commercial-grade iron (CAS No. 7439-89-6, ≥99 %, reduced, powder (fine)) was purchased from Sigma-Aldrich Co., Ltd (Germany). Methylene blue (CAS No. 61-73-4) was purchased from Tianjin Guangfu Fine Chemical Research Institution (Tianjin, China). Methanol (CAS No. 67-56-1) and tert-butanol (CAS No. 75-65-0) were purchased from Fuchen (Tianjin) Chemical Reagents Co., Ltd (China). Sodium persulfate (CAS NO. 7775-27-1) and the other reagents used in this study were obtained from Xilong Scientific

BET

An automatic specific surface area analyzer (ASAP, 2020; Micromeritics, USA) was used to determine the BET surface area of the composite from the nitrogen adsorption isotherm at −196 °C. The BET parameters are shown in Table 1. The BET specific surface area of the present composite was less than that obtained via our previous three-step process (Wu et al., 2020b). Atta-Obeng et al. (2017) indicated that lignin cannot be easily hydrothermally carbonized until 350 °C. We speculate that this may

Conclusion

In this study, we fabricated a MC from waste cartons via one-step hydrothermal conversion, and compared its performance for the activating of PS against that of Pre-ZVI. Both MC/PS and Pre-ZVI/PS treatments could be efficient ways of removing MB. The MB removal efficiency of the Pre-ZVI/PS process reached nearly 90 %, while that of the MC/PS process approached 100 %. After two cycles of magnetic separation, the MC/PS system still achieved rapid and effective decoloration and COD removal for MB.

Author contribution

Yang Wu: Conceptualization, Methodology, Software, Validation, Project administration, Writing - review & editing, Funding acquisition. Xin Fang: Methodology, Writing - original draft, Formal analysis. Xiang-Tian Yang: Methodology, Writing - original draft. Chung-Yu Guan: Supervision, Validation, Writing - review & editing. Xin-Ru Sun: Software. Hong-Yu Wu: Software. Anyi Hu: Methodology, Funding acquisition. Li-Feng Lin: Resources. Qing-Qing Xiao: Resources.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence this publication.

Acknowledgements

This work was supported by Open Fund of the Key Laboratory of Urban Pollutant Conversion, Chinese Academy of Sciences (KLUPC-KF-2020-3), the Anhui Provincial Natural Science Foundation (grant number 1908085ME170), the National Science Foundation of China (grant number 31870475), and Domestic Visiting Project for Youth Talent in Universities of Anhui Province in 2021 (gxgnfx2021160). We are grateful to Ms. Jiani Wang for the XRD measurements.

References (47)

  • Z. Jiang et al.

    Removal of atrazine by biochar-supported zero-valent iron catalyzed persulfate oxidation: reactivity, radical production and transformation pathway

    Environ. Res.

    (2020)
  • N. Kataria et al.

    Application of EDTA modified Fe3O4/sawdust carbon nanocomposites to ameliorate methylene blue and brilliant green dye laden water

    Environ. Res.

    (2019)
  • L. Liu et al.

    Comparative study on treatment of methylene blue dye wastewater by different internal electrolysis systems and COD removal kinetics, thermodynamics and mechanism

    Chemosphere

    (2020)
  • Y. Liu et al.

    Enhanced catalytic degradation of methylene blue by α-Fe2O3/graphene oxide via heterogeneous photo-Fenton reactions

    Appl. Catal. B Environ.

    (2017)
  • H. Meng et al.

    Insight into the effect of lignocellulosic biomass source on the performance of biochar as persulfate activator for aqueous organic pollutants remediation: epicarp and mesocarp of citrus peels as examples

    J. Hazard Mater.

    (2020)
  • G.D.R. Nogueira et al.

    Hydrothermal carbonization of acerola (Malphigia emarginata D.C.) wastes and its application as an adsorbent

    Waste Manag.

    (2019)
  • Y. Pan et al.

    Enhanced degradation of Rhodamine B by pre-magnetized Fe0/PS process: parameters optimization, mechanism and interferences of ions

    Separ. Purif. Technol.

    (2018)
  • Y. Qi et al.

    Three-dimensional porous graphene-like biochar derived from Enteromorpha as a persulfate activator for sulfamethoxazole degradation: role of graphitic N and radicals transformation

    J. Hazard Mater.

    (2020)
  • Y. Qiu et al.

    Contribution of different iron species in the iron-biochar composites to sorption and degradation of two dyes with varying properties

    Chem. Eng. J.

    (2020)
  • P. Salimi et al.

    Two-step synthesis of nanohusk Fe3O4 embedded in 3D network pyrolytic marine biochar for a new generation of anode materials for Lithium-Ion batteries

    J. Alloys Compd.

    (2019)
  • Y. Shi et al.

    Activation of persulfate by EDTA-2K-derived nitrogen-doped porous carbons for organic contaminant removal: radical and non-radical pathways

    Chem. Eng. J.

    (2020)
  • C. Wang et al.

    Efficient use of waste carton for power generation, tar and fertilizer through direct carbon solid oxide fuel cell

    Renew. Energy

    (2020)
  • M. Wei et al.

    Activation of peroxymonosulfate by graphitic carbon nitride loaded on activated carbon for organic pollutants degradation

    J. Hazard Mater.

    (2016)
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