Citation: Yuanpei ZHANG, Jiahong WANG, Jinming HUANG, Zhi HU. Preparation of magnetic mesoporous carbon loaded nano zero-valent iron for removal of Cr(Ⅲ) organic complexes from high-salt wastewater[J]. Chinese Journal of Inorganic Chemistry, ;2024, 40(9): 1731-1742. doi: 10.11862/CJIC.20240077 shu

Preparation of magnetic mesoporous carbon loaded nano zero-valent iron for removal of Cr(Ⅲ) organic complexes from high-salt wastewater

Yuanpei ZHANG ^{1, 2} ,
Jiahong WANG ^{1, 2,,} ,
Jinming HUANG ^{1, 2} ,
Zhi HU ^{1, 2}

1.
School of Environmental Science and Engineering, Shaanxi University of Science & Technology, Xi'an 710021, China
2.
Shaanxi Key Laboratory of Green Preparation and Functionalization of Inorganic Materials, Xi'an 710021, China

Corresponding author: Jiahong WANG, wangjiahong@sust.edu.cn
Received Date: 11 March 2024
Revised Date: 29 June 2024

Figures(11)

Magnetically mesoporous carbon (Fe₃O₄@C)/nano-zerovalent iron (nZVI) composites (Fe₃O₄@C-nZVI) were successfully prepared by a liquid-phase reduction for the effective removal of Cr(Ⅲ)-EDTA (EDTA: ethylenediaminetetra-acetic acid) in high-salinity wastewater. By characterization and analysis by scanning electron microscope (SEM) and electron microscope (TEM), the nZVI has been successfully loaded into the carbon layer without significant agglomeration and can be magnetically separated and nZVI was stable under the protection of a carbon layer which is favorable for the reuse of materials. The presence of nZVI on the adsorbents greatly improved the adsorption of Cr(Ⅲ)-EDTA and the maximum adsorption capacity of Fe₃O₄@C-nZVI was 10.24 mg·g^-1 at pH=4.0, 25 ℃, which was remarkably higher than that of Fe₃O₄@C (4.31 mg·g^-1). The results showed that the Langmuir model and the pseudo-second-order kinetic model can better describe the adsorption of Cr(Ⅲ)-EDTA by Fe₃O₄@C-nZVI. The adsorption capacity of Fe₃O₄@C-nZVI on Cr(Ⅲ)-EDTA increased and then decreased with the increase of solution pH value; low concentrations of complexing agents (EDTA, citric acid) would promote the adsorption of Cr(Ⅲ)-EDTA, whereas an increase in the concentration of the complexing agents showed inhibition; due to the charge shielding effect, high concentrations of cations (Na⁺, K⁺, Ca²⁺) in the solution will promote the adsorption of Cr(Ⅲ)-EDTA. Fe₃O₄@C-nZVI still showed significant adsorption of Cr(Ⅲ)-EDTA in a salt and complexant environment. The adsorption saturated Fe₃O₄@C-nZVI was regenerated by 0.1 mol·L^-1 HCl solution, the adsorption of Cr(Ⅲ)-EDTA by Fe₃O₄@CnZVI reached 6.90 mg·g^-1 after three regeneration cycles. X -ray photoelectron spectrum analysis of Fe₃O₄@C-nZVI before and after reaction showed that the adsorption mechanism was mainly through complexation between surface FeⅢ and Cr(Ⅲ)-EDTA to form FeⅢ-EDTA-Cr(Ⅲ) complexation products, and subsequently displaces Cr(Ⅲ) due to ionic displacement, and the displaced Cr(Ⅲ) will be removed by co-precipitation with FeⅢ as Cr_xFe_1-x(OH)₃ deposited on the nZVI surface.
- magnetically mesoporous carbon,
- nano zero-valent iron,
- Cr(Ⅲ),
- high salinity water,
- adsorption mechanism
1. [1]
  Wu Z Y, Zhang H, Ali E, Shahab A, Huang H Y, Ullah H, Zeng H H. Synthesis of novel magnetic activated carbon for effective Cr(Ⅵ) removal via synergistic adsorption and chemical reduction[J]. Environ. Technol. Innov., 2023,30103092. doi: 10.1016/j.eti.2023.103092
2. [2]
  Murthy M K, Khandayataray P, Padhiary S, Samal D. A review on chromium health hazards and molecular mechanism of chromium bioremediation[J]. Rev. Environ. Health, 2023,38:461-478. doi: 10.1515/reveh-2021-0139
3. [3]
  YANG S L, CHEN Y H, YAN M L, WEI C T, LI S X, JIA B J. Effect of free water molecule in copper complexes on the performance of light absorption and adsorption of Cr(Ⅵ)[J]. Chinese J. Inorg. Chem., 2023,39(11):2160-2168.
4. [4]
  Mpofu A B, Oyekola O O, Welz P J. Anaerobic treatment of tannery wastewater in the context of a circular bioeconomy for developing countries[J]. J. Clean. Prod., 2021,29626490.
5. [5]
  Ma R G, Wang T, Huang T B, Sun W L, Qiao S, Liu W. Insights into interactions of Cr(Ⅲ) and organic matters during adsorption onto titanate nanotubes: Differential absorbance and DFT study[J]. J. Mol. Liq., 2020,312113432. doi: 10.1016/j.molliq.2020.113432
6. [6]
  HU K, WANG J S, MAO R, LIU Y, WANG K F, ZHANG R S, LIU X B, SHI D Z, ZHAO X. Enhanced decomplexation of Cu-EDTA and cathode recovery of Cu by the Fenton-like oxidation using pulsed[J]. Acta Scientiae Circumstantiae, 2023,43(12):354-364.
7. [7]
  Lu K Q, Gao M M, Sun B, Wang M, Wang S G, Wang X H. Simultaneous removal of Cr and organic matters via coupling Cr-Fenton-like reaction with Cr flocculation: The key role of Cr flocs on coupling effect[J]. Chemosphere, 2022,287131991. doi: 10.1016/j.chemosphere.2021.131991
8. [8]
  Anfar Z, Ahsaine H A, Zbair M, Amedlous A, El Fakir A A, Jada A, El Alem N. Recent trends on numerical investigations of response surface methodology for pollutants adsorption onto activated carbon materials: A review[J]. Crit. Rev. Environ. Sci. Technol., 2019,50:1043-1084.
9. [9]
  LUO Z Y, LIU C, HUANG L, SHEN J Y, WANG Z X. The research and application progress of heavy metal capturing agents in water treatment a review[J]. Environmental Pollution & Control, 2022,44(11):1519-1525.
10. [10]
  Xia X, Yang J J, Yan Y B, Wang J, Hu Y F, Zeng X B. Molecular sorption mechanisms of Cr(Ⅲ) to organo-ferrihydrite coprecipitates using synchrotron-based EXAFS and STXM techniques[J]. Environ. Sci. Technol., 2020,54:12989-12997. doi: 10.1021/acs.est.0c02872
11. [11]
  Benzigar M R, Talapaneni S N, Joseph S, Ramadass K, Singh G, Scaranto J, Ravon U, Al-Bahily K, Vinu A. Recent advances in functionalized micro and mesoporous carbon materials: Synthesis and applications[J]. Chem. Soc. Rev., 2018,47:2680-2721. doi: 10.1039/C7CS00787F
12. [12]
  Wang B L, Fu Y G, Li J, Liu T. Yolk-shelled Co@SiO₂@mesoporous carbon microspheres: Construction of multiple heterogeneous interfaces for wide-bandwidth microwave absorption[J]. J. Colloid Interface Sci., 2022,607:540-1550.
13. [13]
  WANG F, TAN X P, LIAO B, LIU Z, PENG Q A, ZHU C N. Review on remediation of soil heavy metal pollution by nanoscale zero-valent iron[J]. Applied Chemical Industry, 2023,52(4):1257-1263.
14. [14]
  LIU Z X, KE Y, HUANG L, JI L L, ZHANG W C, WANG T Y. Advances in the modification and application of nanoscale zero-valent iron[J]. New Chemical Materials, 2023,51(12):253-259.
15. [15]
  ZHU J L, GUO S C, XU W J, FENG Y C, CAI Q, NI Y C, SUN R. Preparation of nano iron-modified biochar and its adsorption performance on chromium-containing wastewater[J]. Chinese Journal of Environmental Engineering, 2023,17(9):2891-2898.
16. [16]
  Dong Z C, Xu Y Y, Wu C, Chao J, Chen T. Efficient removal of natural organo-chromium(Ⅲ) through self-circulating decomplex and immobilization with nanoscale zero-valent iron[J]. Nano Res., 2024,17:364-371. doi: 10.1007/s12274-023-6028-9
17. [17]
  Liang L Q, Wang J H, Zhang Y X. Magnetic mesoporous carbon hollow microspheres adsorbents for the efficient removal of Cr(Ⅲ) and Cr(Ⅲ)-EDTA in high salinity water[J]. Microporous Mesoporous Mat., 2023,347112344. doi: 10.1016/j.micromeso.2022.112344
18. [18]
  Cheng Y, Zhou W J, Zhu L Z. Enhanced reactivity and mechanisms of mesoporous carbon supported zero-valent iron composite for trichloroethylene removal in batch studies[J]. Sci. Total Environ., 2020,718137256. doi: 10.1016/j.scitotenv.2020.137256
19. [19]
  Zhang S, Lyu H H, Tang J C, Song B R, Zhen M H, Liu X M. A novel biochar supported CMC stabilized nano zero-valent iron composite for hexavalent chromium removal from water[J]. Chemosphere, 2019,217:686-694. doi: 10.1016/j.chemosphere.2018.11.040
20. [20]
  LIU S P, XIA X K, XIN B W, ZHANG Y R, BAI Y, JIN H, LI C W. Study on mechanism of adsorption of Cr(Ⅵ) by modified activated carbon loaded with nano-zero-valent iron[J]. Journal of University of Science and Technology, 2023,46(4):287-295.
21. [21]
  Wu Y W, Chen X T, Han Y, Yue D T, Cao X D, Zhao Y X, Qian X F. Highly efficient utilization of nano-Fe(0) Embedded in mesoporous carbon for activation of peroxydisulfate[J]. Environ. Sci. Technol., 2019,53:9081-9090. doi: 10.1021/acs.est.9b02170
22. [22]
  Ren Y, Abbood H A, He F B, Peng H, Huang K X. Magnetic EDTA-modified chitosan/SiO₂/Fe₃O₄ adsorbent: Preparation, characterization, and application in heavy metal adsorption[J]. Chem. Eng. J., 2013,226:300-311. doi: 10.1016/j.cej.2013.04.059
23. [23]
  Cao X H, Guo J, Mao J D, Lan Y Q. Adsorption and mobility of Cr(Ⅲ)-organic acid complexes in soils[J]. J. Hazard. Mater., 2011,192:1533-1538. doi: 10.1016/j.jhazmat.2011.06.076
24. [24]
  Grzetic D J, Delaney K T, Fredrickson G H. Field-theoretic study of salt-induced order and disorder in a polarizable diblock copolymer[J]. ACS Macro. Lett., 2019,8:962-967. doi: 10.1021/acsmacrolett.9b00316
25. [25]
  Zhang Y, Yang M, Dou X M, He H, Wang D S. Arsenate Adsorption on an Fe-Ce bimetal oxide adsorbent: Role of surface properties[J]. Environ. Sci. Technol., 2005,39:7246-7253. doi: 10.1021/es050775d
26. [26]
  Song L, Jing S C, Qiu Y X, Liu F Q, Li A M. Efficient removal of Cr(Ⅲ)-carboxyl complex from neutral and high-salinity wastewater by nitrogen doped biomass-based composites[J]. Chin. Chem. Lett., 2023,34107180. doi: 10.1016/j.cclet.2022.01.073
27. [27]
  Bae S, Hanna K. Reactivity of nanoscale zero-valent iron in unbuffered systems: Effect of pH and Fe(Ⅱ) dissolution[J]. Environ. Sci. Technol., 2015,49(17):10536-10543. doi: 10.1021/acs.est.5b01298
28. [28]
  Liao M Z, Zhao S X, Wei K, Sun H W, Zhang L Z. Precise decomplexation of Cr(Ⅲ)-EDTA and in-situ Cr(Ⅲ) removal with oxalated zero-valent iron[J]. Appl. Catal. B-Environ., 2023,330122619. doi: 10.1016/j.apcatb.2023.122619
29. [29]
  Ikemoto I, Ishii K, Kinoshita S, Kuroda H, Alario Franco M A, Thomas J M. X-ray photoelectron spectroscopic studies of CrO₂ and some related chromium compounds[J]. J. Solid State Chem., 1976,17:425-430. doi: 10.1016/S0022-4596(76)80012-6
30. [30]
  Esfandiari N, Kashefi M, Mirjalili M, Afsharnezhad S. Role of silica mid-layer in thermal and chemical stability of hierarchical Fe₃O₄-SiO₂-TiO₂ nanoparticles for improvement of lead adsorption: Kinetics, thermodynamic and deep XPS investigation[J]. Mater. Sci. Eng. B, 2020,262114690. doi: 10.1016/j.mseb.2020.114690
31. [31]
  Niu Q J, Liu M L, Fang L Y, Yu Y Y, Cheng L, You T L. Highly dispersed and stable nano zero-valent iron doped electrospun carbon nanofiber composite for aqueous hexavalent chromium removal[J]. RSC Adv., 2022,12:8178-8187. doi: 10.1039/D2RA00193D
32. [32]
  HUA Y L, LI D H, GU T H, WANG W, LI R F, YANG J P, ZHANG W X. Enrichment of uranium from aqueous solutions with nanoscale zero-valent iron: Surface chemistry and application prospect[J]. Acta Chim. Sin., 2021,79(8):1008-1022.
33. [33]
  ZHANG C A, JIN L, HUANG Y P, TIAN H L, CAO X Q, FANG Y F. Anti-oxidation ability of nanoscale zero valent iron viaacetone flushing method[J]. Environmental Chemistry, 2021,40(3):790-798.
34. [34]
  Wang S, Gao B, Li Y, Creamer A E, He F. Adsorptive removal of arsenate from aqueous solutions by biochar supported zero-valent iron nanocomposite: Batch and continuous flow tests[J]. J. Hazard. Mater., 2022,322:172-181.
35. [35]
  Zhang S J, Li X Y, Chen J P. An XPS study for mechanisms of arsenate adsorption onto a magnetite-doped activated carbon fiber[J]. J. Colloid Interface Sci., 2010,343:232-238. doi: 10.1016/j.jcis.2009.11.001
36. [36]
  Roverso M, Di Marco V, Favaro G, Di Gangi I M, Badocco D, Zerlottin M, Refosco D, Tapparo A, Bogialli S, Pastore P. New insights in the slow ligand exchange reaction between Cr(Ⅲ)-EDTA and Fe(Ⅲ), and direct analysis of free and complexed EDTA in tannery wastewaters by liquid chromatography-Tandem mass spectrometry[J]. Chemosphere, 2021,264128487. doi: 10.1016/j.chemosphere.2020.128487
37. [37]
  LI R. Study on the performance and mechanism of heavy metal complexes removal based on iron ions replacement strategy. Nanjing: Nanjing University of Science and Technology, 2022: 44-67
38. [38]
  LONG Y, QIAN L B, LI Y G, ZAHNG W Y, WEI Z F, DONG X Z, YANG L, WU W P, YAN J C, CHEN M F. Mechanism of enhanced removal of Cr(Ⅵ) by acid and alkali modified biochar nanoscale zero-valent iron[J]. Chinese Journal of Environmental Engineering, 2022,16(4):1165-1174.
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