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

Eugeniusz Swistun
Eugeniusz Swistun
, 
Maciej Sobczyk
Maciej Sobczyk
, 
A. Santhana Krishna Kumar
A. Santhana Krishna Kumar
, 
Wei-Lung Tseng
Wei-Lung Tseng
 oraz 
Tomasz Bajda
Tomasz Bajda
   | 16 sie 2023
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Article Category: Original Paper
Data publikacji: 16 sie 2023
Zakres stron: 18 - 30
Otrzymano: 07 lut 2023
Przyjęty: 30 maj 2023
DOI: https://doi.org/10.2478/mipo-2023-0003
Słowa kluczowe
© 2023 Eugeniusz Swistun et al., published by Sciendo
This work is licensed under the Creative Commons Attribution 4.0 International License.

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. Composition XRF [% weight]
1 SiO2 32.05
2 TiO2  0.04
3 Al2O3 27.07
4 Fe2O3  0.40
5 MnO  0.08
6 MgO  1.16
7 CaO  5.32
8 K2O  0.52
9 Na2O  8.81
10 P2O5  0.07
11 SO3  0.10
12 LOI 24.19
Σ 99.81

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

Adsorption material pH qm (mg g-1) Reference
Alginate@Iron-zirconium@Zeolite W 2.0 42.3 Abdellaoui et al. 2021
Chitosan-coated Na–X zeolite 2.0 63.2 Han et al. 2019
Zeolite@nanoscale zero-valent iron 3.0 38.2 Suazo-Hernandez et al. 2019
Na-X zeolite derived from cola fly ash 2.14 27.7 Yang et al. 2019
Nanozero valent iron (NZVI) loaded on zeolite 5A 4-12 72.0 Yang et al. 2022.
β-cyclodextrin modified graphene oxide @ Fe3O4 NPs 4-7.2 99.5 Santhana Krishna Kumar et al. 2017
Iron oxide (hydr) modified zeolite 3.5 1.69 Nekhunguni et al. 2017
Ferric hydroxide microcapsule-loaded alginate beads - 3.80 Sarkar et al. 2010
Calcium alginate beads@methionine magnetic NPs 7-7.5 6.6 Lilhare et al. 2021
Aluminum(III) exchange synthetic zeolite 3-10 10.5 Xu et al. 2002
Fe-treated synthetic zeolite - 22.5 Dousova et al. 2006
Cerium(III) exchange synthetic zeolite - 23.4 Haron et al. 2008
Synthetic zeolites 3.2 35.8 Chutia et al. 2009
PEI-modified zeolite beads 5-7.5 35.4 This study
PEI-modified Fe3O4 beads 5-7.5 88.4 This study
Fe3O4 decorated PEI-modified zeolite beads 5-7.5 163.9 This study

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

Sl. No Adsorbent Order of kinetics Characteristic values Uptake of As(V) Uptake of Vanadium(V)
1 PEI-modified zeolite beads Pseudo first order qe (mg g-1) 1.36 1.28
k1 0.007 0.018
Adj. R2 0.92 0.94
2 PEI-modified zeolite beads Pseudo second order qe (mg g-1) 28.4 23.2
k2 0.0005 0.0008
Adj R2 0.98 0.98
3 PEI-modified Fe3O4 beads Pseudo second order qe (mg g-1) 67.1 46.5
k2 0.0002 0.0004
Adj R2 0.98 0.98
4 PEI-modified Fe3O4 beads Pseudo first order qe (mg g-1) 1.66 1.58
k1 0.016 0.019
Adj. R2 0.96 0.94
5 Fe3O4 decorated PEI-modified Pseudo first order qe (mg g-1) 1.86 1.72
zeolite beads k1 0.014 0.02
Adj. R2 0.94 0.94
6 Fe3O4 decorated PEI-modified Pseudo second order qe (mg g-1) 99.0 77.5
zeolite beads k2 0.0001 0.0002
Adj R2 0.98 0.98

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

Sl. No. Adsorbent Isotherm Characteristic values Uptake of As(V) Uptake of V(V)
1 PEI-modified zeolite beads Langmuir qm (mg g-1) 35.4 38.9
b (L mg-1) 0.014 0.014
RL 0.69 0.69
Adj. R2 0.96 0.96
2 PEI-modified zeolite beads Freundlich KF (mg 1-1/n g-1 L 1/n) 0.40 0.44
n 1.08 1.08
Adj R2 0.98 0.98
3 PEI-modified Fe3O4 beads Freundlich KF (mg1-1/ng-1L1/n) 1.008 0.68
n 1.08 1.02
Adj R2 0.98 0.98
4 PEI-modified Fe3O4 beads Langmuir qm (mg g-1) 88.4 53.1
b (L mg-1) 0.01 0.02
RL 0.57 0.30
Adj. R2 0.96 0.96
5 Fe3O4 decorated PEI-modified zeolite beads Langmuir qm (mg g-1) 163.9 151.5
b (L mg-1) 0.02 0.02
RL 0.25 0.25
Adj. R2 0.96 0.96
6 Fe3O4 decorated PEI-modified zeolite beads Freundlich KF (mg1-1/ng-1L1/n) 2.09 1.93
n 1.08 1.08
Adj R2 0.98 0.98

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

Adsorption material Equilibrium kinetics (Time in min) qm (mg g-1) Reference
Chitosan-coated Na–X zeolite 720 min 63.2 Han et al. 2019
Na-X zeolite derived from cola fly ash 120 min 27.7 Yang et al. 2019
Iron oxide (hydr) modified zeolite 90 min 1.69 Nekhunguni et al. 2017
Calcium alginate beads@Methionine magnetic NPs 110 min 6.6 Lilhare et al. 2021
Aluminum(III) exchange synthetic zeolite 960 min 10.5 Xu et al. 2002
Synthetic zeolites 100 min 35.8 Chutia et al. 2009
PEI-modified zeolite beads 100 min 35.4 This study
PEI-modified Fe3O4 beads 100 min 88.4 This study
Fe3O4 decorated PEI-modified zeolite beads 100 min 163.9 This study

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

Adsorption material Equilibrium kinetics (Time in hours) qm (mg g-1) Ref
Magnetic zeolite–polypyrrole composite 4 hours 74.9 Mthombeni et al. 2016
Goethite 12 hours 8.2 Zhu et al. 2020
Clinoptilolite modified polypyrrole and iron NPs 14 hours 12.0 Mthombeni et al. 2018
Synthesised zero-valent iron modified kaloin 2 hours 15.0 Bello et al. 2019
PGTFS-NH3+Cl- 4 hours 45.9 Anirudhan et al. 2010
PEI-modified zeolite beads 1.5 hours 38.9 This study
PEI-modified Fe3O4 beads 1.5 hours 53.1 This study
Fe3O4 decorated PEI-modified zeolite beads 1.5 hours 151.5 This study

Vanadium adsorption capacity of various adsorbents reported in the literature.

Adsorption material pH qm (mg g-1) Reference
LDH supported nanoscale zero valent iron 3.0 93.7 Kong et al. 2020
Magnetic zeolite–polypyrrole composite 4-5 74.9 Mthombeni et al. 2016
Syrian natural zeolite 6.0 40.0 Salman et al. 2017
Goethite 4-8 8.2 Zhu et al. 2020
Clinoptilolite modified polypyrrole and iron oxide NPs 4.5 12.0 Mthombeni et al. 2018
Synthesised zero-valent iron modified kaloin 5.0 15.0 Bello et al. 2019
Octylamine functionalized magnetite NPs 3.2 25.7 Parijaee et al. 2014
Zeolite A 4.5 30.0 Mahmood et al. 2019
PGTFS-NH3+Cl- 6.0 45.9 Anirudhan et al. 2010
Biochar stabilized nano zero-valent iron 2-10 48.5 Fan et al. 2020
Metal (hydr)oxide adsorbents 3-4 111.1 Naeem et al. 2007
PEI-modified zeolite beads 5-7.5 38.9 This study
PEI-modified Fe3O4 beads 5-7.5 53.1 This study
Fe3O4 decorated PEI-modified zeolite beads 5-7.5 151.5 This study

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

S. No. Adsorbent Uptake of metals ΔS0 J mol-1 ΔH0 KJ mol-1 ΔG0 KJ mol-1
298K 308K 318K 328K
1 PEI-Zeolite NSs As(V) 145.7 42.5 −2.1245 −3.9625 −5.2465 −6.8752
beads V(V) 124.8 39.1 −1.4523 −2.2754 −3.1465 −4.1254
2 PEI-Fe3O4 NPs As(V) −121.3 −37.2 −6.8875 −5.2354 4.26548 −2.1256
beads V(V) −91.3 −26.7 −4.2810 −3.8965 −2.23689 −1.4689
3 PEI-Zeolite NSs@ As(V) −163.1 −54.8 −8.3567 −7.3658 −5.2136 −2.8969
Fe3O4 NPs beads V(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)
1 472.0 0.222 0.176 0.13
eISSN:
1899-8526
Język:
Angielski
Częstotliwość wydawania:
Volume Open
Dziedziny czasopisma:
Geosciences, Geophysics, other
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