Preparation of nZVI embedded modified mesoporous carbon for catalytic persulfate to degradation of reactive black 5

doi:10.1007/s11783-020-1372-4

Front. Environ. Sci. Eng.

2021, Vol. 15

Issue (5) : 98 https://doi.org/10.1007/s11783-020-1372-4

RESEARCH ARTICLE

Preparation of nZVI embedded modified mesoporous carbon for catalytic persulfate to degradation of reactive black 5

Zhifei Ma¹, Huali Cao¹, Fengchun Lv², Yu Yang², Chen Chen², Tianxue Yang², Haixin Zheng¹, Daishe Wu¹(

)

¹. Key Laboratory of Poyang Lake Environment and Resource Utilization (Ministry of Education), School of Resources Environmental & Chemical Engineering, Nanchang University, Nanchang 330031, China
². State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China

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Abstract

• The MCNZVI is prepared as an interesting material for PS activation.

• Graphitized carbon shells facilitate electron transfer from Fe⁰.

• The MCNZVI exhibits excellent performance to degrade RB5 by ¹O₂.

• The MCNZVI has high stability and reusability in the oxidation system.

High-efficiency and cost-effective catalysts with available strategies for persulfate (PS) activation are critical for the complete mineralization of organic contaminants in the environmental remediation and protection ﬁelds. A nanoscale zero-valent iron-embedded modified mesoporous carbon (MCNZVI) with a core-shell structure is synthesized using the hydrothermal synthesis method and high-temperature pyrolysis. The results showed that nZVI could be impregnated within mesoporous carbon frameworks with a comparatively high graphitization degree, rich nitrogen doping content, and a large surface area and pore volume. This material was used as a persulfate activator for the oxidation removal of Reactive Black 5 (RB5). The effects of the material dosage, PS concentration, pH, and some inorganic anions (i.e., Cl⁻, SO₄²⁻) on RB5 degradation were then investigated. The highest degradation efficiency (97.3%) of RB5 was achieved via PS (20 mmol/L) activation by the MCNZVI (0.5 g/L). The pseudo-ﬁrst-order kinetics (k = 2.11 × 10⁻² min⁻¹) in the MCNZVI/PS (0.5 g/L, 20 mmol/L) was greater than 100 times than that in the MCNZVI and PS. The reactive oxygen species (ROS), including ¹O₂, SO₄^·⁻, HO^·, and ·O₂⁻, were generated by PS activation with the MCNZVI. Singlet oxygen was demonstrated to be the primary ROS responsible for the RB5 degradation. The MCNZVI could be reused and regenerated for recycling. This work provides new insights into PS activation to remove organic contamination.

Keywords MCNZVI Core-shell structure Reactive Black 5 Persulfate Mechanism

Corresponding Author(s): Daishe Wu

Issue Date: 12 January 2021

Cite this article:

Zhifei Ma,Huali Cao,Fengchun Lv, et al. Preparation of nZVI embedded modified mesoporous carbon for catalytic persulfate to degradation of reactive black 5[J]. Front. Environ. Sci. Eng., 2021, 15(5): 98.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1372-4
https://academic.hep.com.cn/fese/EN/Y2021/V15/I5/98

Fig.1 The XRD patterns (a), FIRT (b), XPS (c) and TEM images (d) are shown for before and after the reaction.

Fig.2 Degradation of RB5 by MCNZVI/PS (a), and the pseudo-ﬁrst-order rate constants (b), inﬂuence of the persulfate amount on RB5 degradation (c), and the pseudo-ﬁrst-order rate constants (d). Conditions: Catalyst= 0.50 g/L, PS= 20 mmol/L, RB5= 20 mg/L.

Fig.3 Eﬀects of the initial pH on the persulfate degradation of RB5. Conditions: Catalyst= 0.50 g/L, PS= 20 mmol/L, RB5= 20 mg/L.

Fig.4 The effect of sulfate and chloride ions on the persulfate degradation of RB5. Conditions: Catalyst= 0.50 g/L, PS= 20 mmol/L, RB5= 20 mg/L.

Fig.5 Radical quenching tests under diﬀerent scavengers (a); the effect of carbon material activation PS without iron (b); the iron concentration changes during the reaction (c) and the ¹O₂ quenching test in an anaerobic environment (d). Conditions: Catalyst= 0.50 g/L, PS= 20 mmol/L, RB5= 20 mg/L.

Fig.6 Reusability(a) and regeneration(b) of MCNZVI activated PS in RB5 degradation. Conditions: Catalyst= 0.50 g/L, PS= 20 mmol/L, RB5= 20 mg/L.

1	M Bhaumik, A Maity, V K Gupta (2017). Synthesis and characterization of Fe0/TiO2 nano-composites for ultrasound assisted enhanced catalytic degradation of Reactive Black 5 in aqueous solutions. Journal of Colloid and Interface Science, 506: 403–414 https://doi.org/10.1016/j.jcis.2017.07.016
2	A Brindha, T Sivakumar (2017). Visible active N, S co-doped TiO2 /graphene photocatalysts for the degradation of hazardous dyes. Journal of Photochemistry and Photobiology A Chemistry, 340: 146–156 https://doi.org/10.1016/j.jphotochem.2017.03.010
3	W M Chen, A P Zhang, Z P Gu, Q Li (2018). Enhanced degradation of refractory organics in concentrated landfill leachate by Fe0/H2O2 coupled with microwave irradiation. Chemical Engineering Journal, 354: 680–691 https://doi.org/10.1016/j.cej.2018.08.012
4	Z H Diao, J J Liu, Y X Hu, L J Kong, D Jiang, X R Xu (2017). Comparative study of Rhodamine B degradation by the systems pyrite/H2O2, and pyrite/persulfate: Reactivity, stability, products and mechanism. Separation and Purification Technology, 184: 374–383 https://doi.org/10.1016/j.seppur.2017.05.016
5	X G Duan, K O’Donnell, H Q Sun, Y Wang, S B Wang (2015). Sulfur and nitrogen co-doped graphene for metal-free catalytic oxidation reactions. Small, 11(25): 3036–3044 https://doi.org/10.1002/smll.201403715
6	Y Feng, P H Lee, D Wu, K Shih (2017). Rapid selective circumneutral degradation of phenolic pollutants using peroxymonosulfate–iodide metal-free oxidation: Role of iodine atoms. Environmental Science & Technology, 51(4): 2312–2320 https://doi.org/10.1021/acs.est.6b04528
7	Y Hou, T Huang, Z Wen, S Mao, S Cui, J Chen (2014). Metal-organic framework-derived nitrogen-doped core-shell-structured porous Fe/Fe3C@C nanoboxes supported on graphene sheets for efficient oxygen reduction reactions. Advanced Energy Materials, 4: 140037 https://doi.org/10.1002/aenm.201400337
8	R L Johnson, J T Nurmi, G S O’Brien Johnson, D Fan, R L O’Brien Johnson, Z Shi, A J Salter-Blanc, P G Tratnyek, G V Lowry (2013). Field-scale transport and transformation of carboxymethylcellulose-stabilized nano zero-valent Iron. Environmental Science & Technology, 47(3): 1573–1580 https://doi.org/10.1021/es304564q
9	R Khaghani, B Kakavandi, K Ghadirinejad, E Dehghani Fard, A Asadi (2019). Preparation, characterization and catalytic potential of g-Fe2O3@AC mesoporous heterojunction for activation of peroxymonosulfate into degradation of cyﬂuthrin insecticide. Microporous and Mesoporous Materials, 284: 111–121 https://doi.org/10.1016/j.micromeso.2019.04.013
10	S Khan, X He, J A Khan, H M Khan, D L Boccelli, D D Dionysiou (2017). Kinetics and mechanism of sulfate radical- and hydroxyl radical-induced degradation of highly chlorinated pesticide lindane in UV/peroxymonosulfate system. Chemical Engineering Journal, 318: 135–142 https://doi.org/10.1016/j.cej.2016.05.150
11	R Khosravi, S Hazrati, M Fazlzadeh (2016). Decolorization of AR18 dye solution by electrocoagulation: Sludge production and electrode loss in different current densities. Desalination and Water Treatment, 57(31): 14656–14664 https://doi.org/10.1080/19443994.2015.1063092
12	M H Kim, C H Hwang, S B Kang, S Kim, S W Park, Y S Yun, S W Won (2015). Removal of hydrolyzed Reactive Black 5 from aqueous solution using a polyethylenimine–polyvinyl chloride composite fiber. Chemical Engineering Journal, 280: 18–25 https://doi.org/10.1016/j.cej.2015.05.069
13	D Li, X Zhu, Y Zhong, W Huang, P Peng (2017). Abiotic transformation of hexabromocyclododecane by sulfidated nanoscale zerovalent iron: kinetics, mechanism and influencing factors. Water Research, 121: 140–149 https://doi.org/10.1016/j.watres.2017.05.019
14	H Li, J Wan, Y Ma, Y Wang, M Huang (2014). Influence of particle size of zero–valent iron and dissolved silica on the reactivity of activated persulfate for degradation of Acid Orange 7. Chemical Engineering Journal, 237: 487–496 https://doi.org/10.1016/j.cej.2013.10.035
15	K K Li, H S Li, T F Xiao, G S Zhang, A P Liang, P Zhang, L H Lin, Z X Chen, X Y Cao, J Y Long (2020). Zero-valent manganese nanoparticles coupled with different strong oxidants for thallium removal from wastewater. Frontiers of Environmental Science & Engineering, 14(2): 34 https://doi.org/10.1007/s11783-019-1213-5
16	P Liang, C Zhang, X Duan, H Sun, S Liu, M O Tade, S Wang(2017). An insight into metal organic framework derived N-doped graphene for the oxidative degradation of persistent contaminants: Formation mechanism and generation of singlet oxygen from peroxymonosulfate. Environmental Science. Nano, 4(2): 315–324 https://doi.org/10.1039/C6EN00633G
17	C Liu, Y P Wang, Y T Zhang, R Li, W D Meng, Z L Song, F Qi, B B Xu, W Chu, D H Yuan, B Yu (2018). Enhancement of Fe@porous carbon to be an efficient mediator for peroxymonosulfate activation for oxidation of organic contaminants: Incorporation NH2-group into structure of its MOF precursor. Chemical Engineering Journal, 354: 835–848 https://doi.org/10.1016/j.cej.2018.08.060
18	W J Ma, N Wang, Y C Du, T Z Tong, L J Zhang, K Y Andrew Lin, X J Han (2019). One-step synthesis of novel Fe3C@nitrogen-doped carbon nanotubes/graphene nanosheets for catalytic degradation of Bisphenol A in the presence of peroxymonosulfate. Chemical Engineering Journal, 356: 1022–1031 https://doi.org/10.1016/j.cej.2018.09.093
19	Z Ma, Y Yang, Y Jiang, B Xi, X Peng, X Y Lian, H Liu (2017). Enhanced degradation of 2,4-dinitrotoluene in groundwater by persulfate activated using iron–carbon micro–electrolysis. Chemical Engineering Journal, 311: 183–190 https://doi.org/10.1016/j.cej.2016.11.083
20	V S Munagapati, V Yarramuthi, Y Kim, K M Lee, D S Kim (2018). Removal of anionic dyes (Reactive Black 5 and Congo Red) from aqueous solutions using Banana Peel Powder as an adsorbent. Ecotoxicology and Environmental Safety, 148: 601–607 https://doi.org/10.1016/j.ecoenv.2017.10.075
21	M H Nie, C X Yan, M Li, X N Wang, W L Bi, W B Dong (2015). Degradation of chloramphenicol by persulfate activated by Fe2+ and zerovalent iron. Chemical Engineering Journal, 279: 507–515 https://doi.org/10.1016/j.cej.2015.05.055
22	H Niu, Y Wang, X Zhang, Z Meng, Y Cai (2012). Easy synthesis of surface-tunable carbon-encapsulated magnetic nanoparticles: Adsorbents for selective isolation and pre-concentration of organic pollutants. ACS Applied Materials & Interfaces, 4(1): 286–295 https://doi.org/10.1021/am201336n
23	A Rahmani, A Shabanloo, M Fazlzadeh, Y Poureshgh, M Vanaeitabar (2019). Optimization of sonochemical decomposition of ciprofloxacin antibiotic in US/PS/NZVI process by CCD-RSM method. Desalination and Water Treatment, 145: 300–308 https://doi.org/10.5004/dwt.2019.23656
24	A Reza Rahmani, A Shabanloo, M Fazlzadeh, Y Poureshgh, H Rezaeivahidian (2016). Degradation of acid blue 113 in aqueous solutions by the electrochemical advanced oxidation in the presence of persulfate. Desalination and Water Treatment, 59: 202–209 https://doi.org/10.5004/dwt.2016.1440
25	A Seid-Mohammadi, A Shabanloo, M Fazlzadeh, Y Poureshgh (2017). Degradation of acid blue 113 by US/H2O2/Fe2+ and US/S2O82–/Fe2+ processes from aqueous solutions. Desalination and Water Treatment, 78: 273–280 https://doi.org/10.5004/dwt.2017.20745
26	P H Shao, X G Duan, J Xu, J Y Tian, W X Shi, S S Gao, M J Xu, F Y Cui, S B Wang (2017). Heterogeneous activation of peroxymonosulfate by amorphous boron for degradation of bisphenol S. Journal of Hazardous Materials, 322: 532–539 https://doi.org/10.1016/j.jhazmat.2016.10.020
27	S Song, L Xu, Z He, J Chen, X Xiao, B Yan (2007). Mechanism of the photocatalytic degradation of C.I. Reactive Black 5 at pH 12.0 using SrTiO3/CeO2 as the catalyst. Environmental Science & Technology, 41(16): 5846–5853 https://doi.org/10.1021/es070224i
28	C P Tso, Y H Shih (2014). The transformation of hexabromocyclododecane using zerovalent iron nanoparticle aggregates. Journal of Hazardous Materials, 277: 76–83 https://doi.org/10.1016/j.jhazmat.2014.04.044
29	S Ullah, X Guo, X Luo, X Zhang, S Leng, N Ma, P Faiz (2020). Rapid and long-effective removal of broad-spectrum pollutants from aqueous system by ZVI/oxidants. Frontiers of Environmental Science & Engineering, 14(5): 89 https://doi.org/10.1007/s11783-020-1268-3
30	Y W Wu, X T Chen, Y Han, D T Yue, X D Cao, Y X Zhao, X F Qian (2019). Highly efficient utilization of nano-Fe0 embedded in mesoporous carbon for activation of peroxydisulfate. Environmental Science & Technology, 53(15): 9081–9090 https://doi.org/10.1021/acs.est.9b02170
31	Y Xie, D M Cwiertny (2010). Use of dithionite to extend the reactive lifetime of nanoscale zero-valent iron treatment systems. Environmental Science & Technology, 44(22): 8649–8655 https://doi.org/10.1021/es102451t
32	J Xu, X R Wang, F Pan, Y Qin, J Xia, J Li, F Wu (2018). Synthesis of the mesoporous carbon-nano-zero-valent iron composite and activation of sulﬁte for removal of organic pollutants. Chemical Engineering Journal, 353: 542–549 https://doi.org/10.1016/j.cej.2018.07.030
33	C Wang, J Kang, P Liang, H Zhang, H Sun, M O Tadé, S Wang (2017). Ferric carbide nanocrystals encapsulated in nitrogen-doped carbon nanotubes as an outstanding environmental catalyst. Environmental Science-Nano, 4:170–179
34	Y Yuan, X S He, B D Xi, D Li, R T Gao, W B Tan, H Zhang, C Yang, X Y Zhao (2018). Polarity and molecular weight of compost-derived humic acid affect Fe(III) oxides reduction. Chemosphere, 208: 77– 83 https://doi.org/10.1016/j.chemosphere.2018.05.160
35	H Zhao, H J Cui, M L Fu (2016). A general and facile method for improving carbon coat on magnetic nanoparticles with a thickness control. Journal of Colloid and Interface Science, 461: 20–24 https://doi.org/10.1016/j.jcis.2015.09.029
36	Z Zhou, X T Liu, K Sun, C Y Lin, J Ma, M C He, W Ouyang (2019). Persulfate-based advanced oxidation processes (AOPs) for organic-contaminated soil remediation: A review. Chemical Engineering Journal, 372: 836–851 https://doi.org/10.1016/j.cej.2019.04.213

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