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Synthetic zeolite derived from coal fly ash decorated with magnetic alginate bead: Application to detoxification of arsenic and vanadium Cover

Synthetic zeolite derived from coal fly ash decorated with magnetic alginate bead: Application to detoxification of arsenic and vanadium

Mineralogia
Volume 54 (2023): Issue 1 (January 2023)
By: Eugeniusz Swistun,  Maciej Sobczyk,  A. Santhana Krishna Kumar,  Wei-Lung Tseng and  Tomasz Bajda  
Open Access
|Aug 2023

Figures & Tables

Figure 1.

Schematic illustration about the synthesis of zeolite NaX-UP.
Schematic illustration about the synthesis of zeolite NaX-UP.

Figure 2.

As shown in (A) PEI-zeolite NSs alginate bead (dusky and colorless), (B) the bare Fe3O4 NPs were decorated on their surface of PEI-zeolite NSs alginate bead (magnetic alginate bead, black color).
As shown in (A) PEI-zeolite NSs alginate bead (dusky and colorless), (B) the bare Fe3O4 NPs were decorated on their surface of PEI-zeolite NSs alginate bead (magnetic alginate bead, black color).

Figure 3.

Schematic illustration for preparation of magnetic alginate bead (adsorbent).
Schematic illustration for preparation of magnetic alginate bead (adsorbent).

Figure 4.

(A) BET adsorption isotherms of NaX-UP zeolites, (B) Pore size distribution of zeolites.
(A) BET adsorption isotherms of NaX-UP zeolites, (B) Pore size distribution of zeolites.

Figure 5.

(A, B, C and D) Powder XRD spectra for (A) NaX-UP zeolite, black line (B) PEI-modified NaX-UP zeolite NSs, brown line; (C) bare Fe3O4 NPs, navy blue line, (D) Fe3O4 NPs decorated PEI-modified NaX-UP zeolite, green line.
(A, B, C and D) Powder XRD spectra for (A) NaX-UP zeolite, black line (B) PEI-modified NaX-UP zeolite NSs, brown line; (C) bare Fe3O4 NPs, navy blue line, (D) Fe3O4 NPs decorated PEI-modified NaX-UP zeolite, green line.

Figure 6.

HR-SEM images and EDS spectra of (A) the bare Fe3O4 NPs were decorated on their surface of PEI-zeolite NSs alginate bead adsorbent, (B and C) after sorption of As(V) & V(V). From (A, B, C) denoted as HR-SEM images, (D, E, F) EDS spectra.
HR-SEM images and EDS spectra of (A) the bare Fe3O4 NPs were decorated on their surface of PEI-zeolite NSs alginate bead adsorbent, (B and C) after sorption of As(V) & V(V). From (A, B, C) denoted as HR-SEM images, (D, E, F) EDS spectra.

Figure 7.

Alginate beads mediated sorption of As(V) and V(V), (A, B) adsorption isotherms modeling of PEI modified NaX-UP zeolite beads, PEI modified Fe3O4 NPs beads, and Fe3O4 NPs decorated PEI modified NaX-UP zeolite beads for (A) As(V) and (B) V(V); adsorption isotherms modeling fitting with the Freundlich model (A: navy blue line; B: dark green line) and Langmuir model (A: cyan line; B: sky blue line). (C, D) Kinetic sorption curves of the PEI modified NaX-UP zeolite beads, PEI modified Fe3O4 NPs beads, and Fe3O4 NPs decorated PEI modified NaX-UP zeolite beads for (C) As(V) and (D) V(V), modeling of kinetics sorption curves with the pseudo-first-order kinetics (C: sky blue line; D: dark yellow line) and pseudo-second-order kinetic (C: dark brown line; D: dark green line). (A, B) Beads-mediated sorption of As (V) and V(V), (C, D) Kinetic sorption curves of As (V) and V(V), PEI-zeolite NSs modified alginate beads, bare Fe3O4 NPs modified alginate beads, and bare Fe3O4NPs decorated on their surface of PEI-zeolite NSs modified alginate beads (1.0 g) were incubated with various concentration of As(V) and V(V) at pH 4.5 for isotherm studies (A, B) and (C, D) the alginate beads were incubated with 50 mg mL-1 of As(V) and V(V) various time interval from 0-240 min at 298 K.
Alginate beads mediated sorption of As(V) and V(V), (A, B) adsorption isotherms modeling of PEI modified NaX-UP zeolite beads, PEI modified Fe3O4 NPs beads, and Fe3O4 NPs decorated PEI modified NaX-UP zeolite beads for (A) As(V) and (B) V(V); adsorption isotherms modeling fitting with the Freundlich model (A: navy blue line; B: dark green line) and Langmuir model (A: cyan line; B: sky blue line). (C, D) Kinetic sorption curves of the PEI modified NaX-UP zeolite beads, PEI modified Fe3O4 NPs beads, and Fe3O4 NPs decorated PEI modified NaX-UP zeolite beads for (C) As(V) and (D) V(V), modeling of kinetics sorption curves with the pseudo-first-order kinetics (C: sky blue line; D: dark yellow line) and pseudo-second-order kinetic (C: dark brown line; D: dark green line). (A, B) Beads-mediated sorption of As (V) and V(V), (C, D) Kinetic sorption curves of As (V) and V(V), PEI-zeolite NSs modified alginate beads, bare Fe3O4 NPs modified alginate beads, and bare Fe3O4NPs decorated on their surface of PEI-zeolite NSs modified alginate beads (1.0 g) were incubated with various concentration of As(V) and V(V) at pH 4.5 for isotherm studies (A, B) and (C, D) the alginate beads were incubated with 50 mg mL-1 of As(V) and V(V) various time interval from 0-240 min at 298 K.

Figure 8.

(A, B, C) Van’t Hoff plot for the adsorption of As (V) and V (V) on the (A) PEI-zeolite NSs modified alginate beads, (B) Fe3O4 NPs modified alginate beads, and (C) Fe3O4 NPs decorated PEI modified zeolite NSs alginate beads. (A-C) The beads-related nanomaterials (1.0 g) were incubated with 50 mg mL-1 of As (V) and V (V) at 298, 308, 318, and 328 K for 0-240 min under pH 7.0 conditions.
(A, B, C) Van’t Hoff plot for the adsorption of As (V) and V (V) on the (A) PEI-zeolite NSs modified alginate beads, (B) Fe3O4 NPs modified alginate beads, and (C) Fe3O4 NPs decorated PEI modified zeolite NSs alginate beads. (A-C) The beads-related nanomaterials (1.0 g) were incubated with 50 mg mL-1 of As (V) and V (V) at 298, 308, 318, and 328 K for 0-240 min under pH 7.0 conditions.

Elemental compositions determined by XRF method_

S. No.CompositionXRF [% weight]
1SiO232.05
2TiO2 0.04
3Al2O327.07
4Fe2O3 0.40
5MnO 0.08
6MgO 1.16
7CaO 5.32
8K2O 0.52
9Na2O 8.81
10P2O5 0.07
11SO3 0.10
12LOI24.19
Σ99.81

Arsenic (V) adsorption capacity of various adsorbents reported in the literature_

Adsorption materialpHqm (mg g-1)Reference
Alginate@Iron-zirconium@Zeolite W2.042.3Abdellaoui et al. 2021
Chitosan-coated Na–X zeolite2.063.2Han et al. 2019
Zeolite@nanoscale zero-valent iron3.038.2Suazo-Hernandez et al. 2019
Na-X zeolite derived from cola fly ash2.1427.7Yang et al. 2019
Nanozero valent iron (NZVI) loaded on zeolite 5A4-1272.0Yang et al. 2022.
β-cyclodextrin modified graphene oxide @ Fe3O4 NPs4-7.299.5Santhana Krishna Kumar et al. 2017
Iron oxide (hydr) modified zeolite3.51.69Nekhunguni et al. 2017
Ferric hydroxide microcapsule-loaded alginate beads-3.80Sarkar et al. 2010
Calcium alginate beads@methionine magnetic NPs7-7.56.6Lilhare et al. 2021
Aluminum(III) exchange synthetic zeolite3-1010.5Xu et al. 2002
Fe-treated synthetic zeolite-22.5Dousova et al. 2006
Cerium(III) exchange synthetic zeolite-23.4Haron et al. 2008
Synthetic zeolites3.235.8Chutia et al. 2009
PEI-modified zeolite beads5-7.535.4This study
PEI-modified Fe3O4 beads5-7.588.4This study
Fe3O4 decorated PEI-modified zeolite beads5-7.5163.9This study

Adsorption kinetics for uptake of Arsenic(V) and Vanadium(V)

Sl. NoAdsorbentOrder of kineticsCharacteristic valuesUptake of As(V)Uptake of Vanadium(V)
1PEI-modified zeolite beadsPseudo first orderqe (mg g-1)1.361.28
k10.0070.018
Adj. R20.920.94
2PEI-modified zeolite beadsPseudo second orderqe (mg g-1)28.423.2
k20.00050.0008
Adj R20.980.98
3PEI-modified Fe3O4 beadsPseudo second orderqe (mg g-1)67.146.5
k20.00020.0004
Adj R20.980.98
4PEI-modified Fe3O4 beadsPseudo first orderqe (mg g-1)1.661.58
k10.0160.019
Adj. R20.960.94
5Fe3O4 decorated PEI-modifiedPseudo first orderqe (mg g-1)1.861.72
zeolite beads k10.0140.02
Adj. R20.940.94
6Fe3O4 decorated PEI-modifiedPseudo second orderqe (mg g-1)99.077.5
zeolite beads k20.00010.0002
Adj R20.980.98

Adsorption isotherm parameters for uptake of Arsenic(V) and Vanadium(V)_

Sl. No.AdsorbentIsothermCharacteristic valuesUptake of As(V)Uptake of V(V)
1PEI-modified zeolite beadsLangmuirqm (mg g-1)35.438.9
b (L mg-1)0.0140.014
RL0.690.69
Adj. R20.960.96
2PEI-modified zeolite beadsFreundlichKF (mg 1-1/n g-1 L 1/n)0.400.44
n1.081.08
Adj R20.980.98
3PEI-modified Fe3O4 beadsFreundlichKF (mg1-1/ng-1L1/n)1.0080.68
n1.081.02
Adj R20.980.98
4PEI-modified Fe3O4 beadsLangmuirqm (mg g-1)88.453.1
b (L mg-1)0.010.02
RL0.570.30
Adj. R20.960.96
5Fe3O4 decorated PEI-modified zeolite beadsLangmuirqm (mg g-1)163.9151.5
b (L mg-1)0.020.02
RL0.250.25
Adj. R20.960.96
6Fe3O4 decorated PEI-modified zeolite beadsFreundlichKF (mg1-1/ng-1L1/n)2.091.93
n1.081.08
Adj R20.980.98

Arsenic (V) equilibrium kinetics sorption, adsorption capacity of various adsorbents reported in the literature_

Adsorption materialEquilibrium kinetics (Time in min)qm (mg g-1)Reference
Chitosan-coated Na–X zeolite720 min63.2Han et al. 2019
Na-X zeolite derived from cola fly ash120 min27.7Yang et al. 2019
Iron oxide (hydr) modified zeolite90 min1.69Nekhunguni et al. 2017
Calcium alginate beads@Methionine magnetic NPs110 min6.6Lilhare et al. 2021
Aluminum(III) exchange synthetic zeolite960 min10.5Xu et al. 2002
Synthetic zeolites100 min35.8Chutia et al. 2009
PEI-modified zeolite beads100 min35.4This study
PEI-modified Fe3O4 beads100 min88.4This study
Fe3O4 decorated PEI-modified zeolite beads100 min163.9This study

Vanadium equilibrium kinetics sorption, adsorption capacity of various adsorbents reported in the literature_

Adsorption materialEquilibrium kinetics (Time in hours)qm (mg g-1)Ref
Magnetic zeolite–polypyrrole composite4 hours74.9Mthombeni et al. 2016
Goethite12 hours8.2Zhu et al. 2020
Clinoptilolite modified polypyrrole and iron NPs14 hours12.0Mthombeni et al. 2018
Synthesised zero-valent iron modified kaloin2 hours15.0Bello et al. 2019
PGTFS-NH3+Cl-4 hours45.9Anirudhan et al. 2010
PEI-modified zeolite beads1.5 hours38.9This study
PEI-modified Fe3O4 beads1.5 hours53.1This study
Fe3O4 decorated PEI-modified zeolite beads1.5 hours151.5This study

Vanadium adsorption capacity of various adsorbents reported in the literature_

Adsorption materialpHqm (mg g-1)Reference
LDH supported nanoscale zero valent iron3.093.7Kong et al. 2020
Magnetic zeolite–polypyrrole composite4-574.9Mthombeni et al. 2016
Syrian natural zeolite6.040.0Salman et al. 2017
Goethite4-88.2Zhu et al. 2020
Clinoptilolite modified polypyrrole and iron oxide NPs4.512.0Mthombeni et al. 2018
Synthesised zero-valent iron modified kaloin5.015.0Bello et al. 2019
Octylamine functionalized magnetite NPs3.225.7Parijaee et al. 2014
Zeolite A4.530.0Mahmood et al. 2019
PGTFS-NH3+Cl-6.045.9Anirudhan et al. 2010
Biochar stabilized nano zero-valent iron2-1048.5Fan et al. 2020
Metal (hydr)oxide adsorbents3-4111.1Naeem et al. 2007
PEI-modified zeolite beads5-7.538.9This study
PEI-modified Fe3O4 beads5-7.553.1This study
Fe3O4 decorated PEI-modified zeolite beads5-7.5151.5This study

Adsorption of thermodynamics for uptake of As(V) and V(V)_

S. No.AdsorbentUptake of metalsΔS0 J mol-1ΔH0 KJ mol-1ΔG0 KJ mol-1
298K308K318K328K
1PEI-Zeolite NSsAs(V)145.742.5−2.1245−3.9625−5.2465−6.8752
beadsV(V)124.839.1−1.4523−2.2754−3.1465−4.1254
2PEI-Fe3O4 NPsAs(V)−121.3−37.2−6.8875−5.23544.26548−2.1256
beadsV(V)−91.3−26.7−4.2810−3.8965−2.23689−1.4689
3PEI-Zeolite NSs@As(V)−163.1−54.8−8.3567−7.3658−5.2136−2.8969
Fe3O4 NPs beadsV(V)−126.4−50.3−5.1209−3.6875−1.4232−2.0256

Surface area, pore volume and pore diameter of NaX-UP zeolites_

S. No.SBET (m2 g-1)Vtot0.99 (cm3 g-1)VmikDR (cm3 g-1)VmezBJH (cm3 g-1)
1472.00.2220.1760.13
DOI: https://doi.org/10.2478/mipo-2023-0003 | Journal eISSN: 1899-8526 | Journal ISSN: 1899-8291
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Language: English
Page range: 18 - 30
Submitted on: Feb 7, 2023
Accepted on: May 30, 2023
Published on: Aug 16, 2023
Published by: Mineralogical Society of Poland
In partnership with: Paradigm Publishing Services
Publication frequency: 1 issue per year
Keywords:
Fly ash,
zeolite,
magnetic nanoparticle,
alginate bead,
electrostatic interaction,
heavy metal sorption
Related subjects:
Geosciences,
Geophysics,
Geosciences, other

© 2023 Eugeniusz Swistun, Maciej Sobczyk, A. Santhana Krishna Kumar, Wei-Lung Tseng, Tomasz Bajda, published by Mineralogical Society of Poland
This work is licensed under the Creative Commons Attribution 4.0 License.

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