Simple Aminated Modified Zeolite 4A Synthesized Using Fly Ash and Its Remediation of Mercury Contamination: Characteristics and Mechanism
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials and Reagents
2.2. Instruments
2.3. Synthesis and Amination Modification of Zeolite 4A
2.3.1. Zeolite 4A Synthesis
2.3.2. Inorganic Amination Modification
2.3.3. Organic Graft Modification
2.4. Adsorption Experiment
2.5. Cation Effect on Hg2+ Ion Adsorption
2.6. Zeolite Reuse Experiment
2.7. Removal of Hg2+ Ions in Soil Leaching by the Modified Zeolite
3. Results
3.1. Amination Modification of Zeolite
3.1.1. Characterization
3.1.2. Synthesis Mechanism
3.1.3. Pore Size Distribution
3.2. Hg2+ Ion Adsorption by Modified Zeolite
3.2.1. Adsorption Efficiency
3.2.2. Effect of Initial Solution pH
3.2.3. Adsorption Model
3.2.4. Adsorption Mechanism
3.3. Coexisting Multiple Ion Effect and Reusability
3.4. Hg2+ Ion Adsorption in Soil Leaching
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
- Mon, M.; Lloret, F.; Ferrando-Soria, J.; Martí-Gastaldo, C.; Armentano, D.; Pardo, E. Selective and Efficient Removal of Mercury from Aqueous Media with the Highly Flexible Arms of a BioMOF. Angew. Chem. Int. Ed. 2016, 55, 11167–11172. [Google Scholar] [CrossRef] [PubMed]
- Ma, L.; Islam, S.; Xiao, C.; Zhao, J.; Liu, H.; Yuan, M.; Sun, G.; Li, H.; Ma, S.; Kanatzidis, M. Rapid simultaneous removal of toxic anions [HSeO3], [SeO3]2, and [SeO4]2, and metals Hg2+, Cu2+, and Cd2+ by MoS42 intercalated layered double hydroxide. J. Am. Chem. Soc. 2017, 139, 12745–12757. [Google Scholar] [CrossRef]
- Bolisetty, S.; Peydayesh, M.; Mezzenga, R. Sustainable technologies for water purification from heavy metals: Review and analysis. Chem. Soc. Rev. 2019, 48, 463–487. [Google Scholar] [CrossRef] [PubMed]
- Chojnacki, A.; Chojnacka, K.; Hoffmann, J.; Górecki, H. The application of natural zeolites for mercury removal: From laboratory tests to industrial scale. Miner. Eng. 2004, 17, 933–937. [Google Scholar] [CrossRef]
- Murukutti, M.K.; Jena, H. Synthesis of nano-crystalline zeolite-A and zeolite-X from Indian coal fly ash, its characterization and performance evaluation for the removal of Cs+ and Sr2+ from simulated nuclear waste. J. Hazard. Mater. 2021, 423, 127085. [Google Scholar] [CrossRef]
- Belviso, C. State-of-the-art applications of fly ash from coal and biomass: A focus on zeolite synthesis processes and issues. Prog. Energy Combust. Sci. 2018, 65, 109–135. [Google Scholar] [CrossRef]
- Yang, H.-M.; Jeon, H.; Lee, Y.; Choi, M. Sulfur-modified zeolite A as a low-cost strontium remover with improved selectivity for radioactive strontium. Chemosphere 2022, 299, 134309. [Google Scholar] [CrossRef] [PubMed]
- Zhou, G.; Wang, Y.; Zhou, R.; Wang, C.; Jin, Y.; Qiu, J.; Hua, C.; Cao, Y. Synthesis of amino-functionalized bentonite/CoFe2O4@MnO2 magnetic recoverable nanoparticles for aqueous Cd2+ removal. Sci. Total Environ. 2019, 682, 505–513. [Google Scholar] [CrossRef] [PubMed]
- Jawed, A.; Saxena, V.; Pandey, L.M. Engineered nanomaterials and their surface functionalization for the removal of heavy metals: A review. J. Water Process. Eng. 2020, 33, 101009. [Google Scholar] [CrossRef]
- Srasra, M.; Delsarte, S.; Gaigneaux, E.M. Nitrided Zeolites: A Spectroscopic Approach for the Identification and Quantification of Incorporated Nitrogen Species. J. Phys. Chem. C 2010, 114, 4527–4535. [Google Scholar] [CrossRef]
- Agarwal, V.; Huber, G.W.; Conner, W.C., Jr.; Auerbach, S.M. DFT study of nitrided zeolites: Mechanism of nitrogen substitution in HY and silicalite. J. Catal. 2010, 269, 53–63. [Google Scholar] [CrossRef]
- Wu, G.; Wang, X.; Yang, Y.; Li, L.; Wang, G.; Guan, N. Confirmation of NH species in the framework of nitrogen-incorporated ZSM-5 zeolite by experimental and theoretical studies. Microporous Mesoporous Mater. 2010, 127, 25–31. [Google Scholar] [CrossRef]
- Li, X.; Meng, C.; Meng, Y.; Gu, L.; Chen, Q.; Liu, H. Amino acid modified molecular sieves with different pore size for chiral separation. Colloid Surface A 2019, 581, 123789. [Google Scholar] [CrossRef]
- Kim, K.; Lee, S.; Ryu, J.H.; Lee, K.S.; Lee, W.B. An improved CO2 adsorption efficiency for the zeolites impregnated with the amino group: A molecular simulation approach. Int. J. Greenh. Gas. Con. 2013, 19, 350–357. [Google Scholar] [CrossRef]
- Zhao, A.; Samanta, A.; Sarkar, P.; Gupta, R. Carbon Dioxide Adsorption on Amine-Impregnated Mesoporous SBA-15 Sorbents: Experimental and Kinetics Study. Ind. Eng. Chem. Res. 2013, 52, 6480–6491. [Google Scholar] [CrossRef]
- Tsintskaladze, G.; Eprikashvili, L.; Mumladze, N.; Gabunia, V.; Sharashenidze, T.; Zautashvili, M.; Kordzakhia, T.; Shatakishvili, T. Nitrogenous zeolite nanomaterial and the possibility of its application in agriculture. Ann. Agrar. Sci. 2017, 15, 365–369. [Google Scholar] [CrossRef]
- Ramos-Martinez, V.; Ramirez-Vargas, E.; Medellin-Rodriguez, F.; Ávila-Orta, C.; Gallardo-Vega, C.; Jasso-Salcedo, A.; Andrade-Guel, M. Zeolite 13X modification with gamma-aminobutyric acid (GABA). Microporous Mesoporous Mater. 2019, 295, 109941. [Google Scholar] [CrossRef]
- Wang, Y.; Du, T.; Song, Y.; Che, S.; Fang, X.; Zhou, L. Amine-functionalized mesoporous ZSM-5 zeolite adsorbents for carbon dioxide capture. Solid State Sci. 2017, 73, 27–35. [Google Scholar] [CrossRef]
- Zhang, W.; Liu, H.; Sun, C.; Drage, T.C.; Snape, C.E. Performance of polyethyleneimine–silica adsorbent for post-combustion CO2 capture in a bubbling fluidized bed. Chem. Eng. J. 2014, 251, 293–303. [Google Scholar] [CrossRef]
- Sandhu, N.K.; Pudasainee, D.; Sarkar, P.; Gupta, R. Steam Regeneration of Polyethylenimine-Impregnated Silica Sorbent for Postcombustion CO2 Capture: A Multicyclic Study. Ind. Eng. Chem. Res. 2016, 55, 2210–2220. [Google Scholar] [CrossRef]
- Yang, L.; Qian, X.; Yuan, P.; Bai, H.; Miki, T.; Men, F.; Li, H.; Nagasaka, T. Green synthesis of zeolite 4A using fly ash fused with synergism of NaOH and Na2CO3. J. Clean. Prod. 2018, 212, 250–260. [Google Scholar] [CrossRef]
- Ikeda, T.; Yoshida, Y.; Nakazawa, N.; Inagaki, S.; Kubota, Y. Solid-state NMR and powder X-ray diffraction studies on ammonium ion-exchanged and dealuminated zeolite YNU-5. Microporous Mesoporous Mater. 2020, 302, 110197. [Google Scholar] [CrossRef]
- Zhang, C.; Yu, J.; Cao, Z.; Wang, R.; Du, W.; He, P.; Ge, Y. Preparation and properties of silane coupling agent modified zeolite as warm mix additive. Constr. Build. Mater. 2020, 244, 118408. [Google Scholar] [CrossRef]
- Li, Y.; Yang, L.; Li, X.; Miki, T.; Nagasaka, T. A composite adsorbent of ZnS nanoclusters grown in zeolite NaA synthesized from fly ash with a high mercury ion removal efficiency in solution. J. Hazard. Mater. 2021, 411, 125044. [Google Scholar] [CrossRef] [PubMed]
- Zhou, L.; Liu, Z.; Liu, J.; Huang, Q. Adsorption of Hg(II) from aqueous solution by ethylenediamine-modified magnetic crosslinking chitosan microspheres. Desalination 2010, 258, 41–47. [Google Scholar] [CrossRef]
- Falter, R.; Schöler, H.F. Determination of mercury species in natural waters at picogram level with online RP C18 preconcentration and HPLC-UV-PCO-CVAAS. Fresenius J. Anal. Chem. 1995, 353, 34–38. [Google Scholar] [CrossRef]
- Laperdina, T.; Melnikova, M.; Koval, A.; Sidorov, Y.; Nagorny, V.; Ostapchuk, V. Gold mining in Siberia and the Far East as a source of mercury contamination of the environment. J. Environ. Sci. 2000, 12, 51–58. [Google Scholar]
- Zhang, S.; Zhang, Y.; Liu, J.; Xu, Q.; Xiao, H.; Wang, X.; Xu, H.; Zhou, J. Thiol modified Fe3O4@SiO2 as a robust, high effective, and recycling magnetic sorbent for mercury removal. Chem. Eng. J. 2013, 226, 30–38. [Google Scholar] [CrossRef] [Green Version]
- Yang, L.; Li, S.; Wen, T.; Meng, F.; Chen, G.; Qian, X. Influence of ferrous-metal production on mercury contamination and fractionation in farmland soil around five typical iron and steel enterprises of Tangshan, China. Ecotoxicol. Environ. Saf. 2019, 188, 109774. [Google Scholar] [CrossRef]
- Wang, P.; Sun, Q.; Zhang, Y.; Cao, J. Effective removal of methane using nano-sized zeolite 4A synthesized from kaolin. Inorg. Chem. Commun. 2019, 111, 107639. [Google Scholar] [CrossRef]
- Amooghin, A.; Omidkhah, M.; Kargari, A. The effects of aminosilane grafting on NaY zeolite–Matrimid®5218 mixed matrix membranes for CO2/CH4 separation. J. Membr. Sci. 2015, 490, 364–379. [Google Scholar] [CrossRef]
- Purnomo, C.; Salim, C.; Hinode, H. Synthesis of pure Na–X and Na–A zeolite from bagasse fly ash. Micropor. Mesopor. Mater. 2012, 162, 6–13. [Google Scholar] [CrossRef]
- Mahata, B.K.; Chung, K.-L.; Chang, S.-M. Removal of ammonium nitrogen (NH4+-N) by Cu-loaded amino-functionalized adsorbents. Chem. Eng. J. 2021, 411, 128589. [Google Scholar] [CrossRef]
- Kawano, A.; Moteki, T.; Ogura, M. Effect of delamination on active base site formation over nitrided MWW-type zeolite for Knoevenagel condensation. Microporous Mesoporous Mater. 2020, 299, 110104. [Google Scholar] [CrossRef]
- Liu, Y.; Liu, J.; Yao, W.; Cen, W.; Wang, H.; Weng, X.; Wu, Z. The effects of surface acidity on CO2 adsorption over amine functionalized protonated titanate nanotubes. RSC Adv. 2013, 3, 18803–18810. [Google Scholar] [CrossRef]
- Drage, T.; Arenillas, A.; Smith, K.; Snape, C. Thermal stability of polyethylenimine based carbon dioxide adsorbents and its influence on selection of regeneration strategies. Microporous Mesoporous Mater. 2008, 116, 504–512. [Google Scholar] [CrossRef]
- Xu, X.; Zheng, Y.; Gao, B.; Cao, X. N-doped biochar synthesized by a facile ball-milling method for enhanced sorption of CO2 and reactive red. Chem. Eng. J. 2019, 368, 564–572. [Google Scholar] [CrossRef]
- Zendehdel, M.; Bodaghifard, M.A.; Behyar, H.; Mortezaei, Z. Alkylaminopyridine-grafted on HY Zeolite: Preparation, characterization and application in synthesis of 4H-Chromenes. Microporous Mesoporous Mater. 2018, 266, 83–89. [Google Scholar] [CrossRef]
- Diôgo, P.; Francisco, W.; Pedro, A.; Allyson, G.; Rodrigo, S.; Enrique, R.; Diana, C. CO2 adsorption in amine-grafted zeolite 13X. Appl. Surf. Sci. 2014, 314, 314–321. [Google Scholar]
- Chen, Y.; Zhao, Y. Synthesis and characterization of polyacrylonitrile-2-amino-2-thiazoline resin and its sorption behaviors for noble metal ions. React. Funct. Polym. 2003, 55, 89–98. [Google Scholar] [CrossRef]
- Xiong, C.; Li, Y.; Wang, G.; Fang, L.; Zhou, S.; Yao, C.; Chen, Q.; Zheng, X.; Qi, D.; Fu, Y.; et al. Selective removal of Hg(II) with polyacrylonitrile-2-amino-1,3,4-thiadiazole chelating resin: Batch and column study. Chem. Eng. J. 2015, 259, 257–265. [Google Scholar] [CrossRef]
- Monier, M.; Abdel-Latif, D.A. Modification and characterization of PET fibers for fast removal of Hg(II), Cu(II) and Co(II) metal ions from aqueous solutions. J. Hazard. Mater. 2013, 250, 122–130. [Google Scholar] [CrossRef] [PubMed]
- Puspitasari, T.; Kadja, G.; Radiman, C.L.; Darwis, D.; Mukti, R. Two-step preparation of amidoxime-functionalized natural zeolites hybrids for the removal of Pb2+ ions in aqueous environment. Mater. Chem. Phys. 2018, 216, 197–205. [Google Scholar] [CrossRef]
- Wu, J.; Xu, Z.; Zhang, W.; Lv, L.; Pan, B.; Nie, G.; Li, M.; Du, Q. Application of heterogeneous adsorbents in removal of dimethyl phthalate: Equilibrium and heat. AIChE J. 2010, 56, 2699–2705. [Google Scholar] [CrossRef]
- Yang, L.; Gao, M.; Wei, T.; Nagasaka, T. Synergistic removal of As(V) from aqueous solution by nanozero valent iron loaded with zeolite 5A synthesized from fly ash. J. Hazard. Mater. 2021, 424, 127428. [Google Scholar] [CrossRef]
- Li, S.; Bai, H.; Wang, J.; Jing, X.; Liu, Q.; Zhang, M.; Chen, R.; Liu, L.; Jiao, C. In situ grown of nano-hydroxyapatite on magnetic CaAl-layered double hydroxides and its application in uranium removal. Chem. Eng. J. 2012, 193–194, 372–380. [Google Scholar] [CrossRef]
- Tran, L.; Wu, P.; Zhu, Y.; Liu, S.; Zhu, N. Comparative study of Hg(II) adsorption by thiol- and hydroxyl-containing bifunctional montmorillonite and vermiculite. Appl. Sur. Sci. 2015, 356, 91–101. [Google Scholar] [CrossRef]
- Wan, C.; Xie, Q.; Liu, J.; Liang, D.; Huang, X.; Zhou, H.; Tang, Y.; Liu, D. Pilot-scale combined adsorption columns using activated carbon and zeolite for hazardous trace elements removal from wastewater of entrained-flow coal gasification. Process. Saf. Environ. Prot. 2021, 147, 439–449. [Google Scholar] [CrossRef]
- Wu, Z.; Chen, T.; Liu, H.; Wang, C.; Chen, P.; Chen, D.; Xie, J. An insight into the comprehensive application of opal-palygorskite clay: Synthesis of 4A zeolite and uptake of Hg2+. Appl. Clay Sci. 2018, 165, 103–111. [Google Scholar] [CrossRef]
- Czarna, D.; Baran, P.; Kunecki, P.; Panek, R.; Zmuda, R.; Wdowin, M. Synthetic zeolites as potential sorbents of mercury from wastewater occurring during wet FGD processes of flue gas. J. Clean. Prod. 2018, 172, 2636–2645. [Google Scholar] [CrossRef]
- Sun, Y.; Lv, D.; Zhou, J.; Zhou, X.; Lou, Z.; Baig, S.A.; Xu, X. Adsorption of mercury (II) from aqueous solutions using FeS and pyrite: A comparative study. Chemosphere 2017, 185, 452–461. [Google Scholar] [CrossRef] [PubMed]
- Xu, L.; Liu, Y.; Wang, J.; Tang, Y.; Zhang, Z. Selective adsorption of Pb2+ and Cu2+ on amino-modified attapulgite: Kinetic, thermal dynamic and DFT studies. J. Hazard. Mater. 2020, 404, 124140. [Google Scholar] [CrossRef] [PubMed]
- Li, Y.; Zhang, P.; Du, Q.; Peng, X.; Liu, T.; Wang, Z.; Xia, Y.; Zhang, W.; Wang, K.; Zhu, H.; et al. Adsorption of fluoride from aqueous solution by graphene. J. Colloid Interface Sci. 2011, 363, 348–354. [Google Scholar] [CrossRef] [PubMed]
- Freundlich, H. Over the adsorption in solution. J. Phys. Chem. 1906, 57, 385–471. [Google Scholar]
- Ho, Y.; McKay, G. The kinetics of sorption of divalent metal ions onto sphagnum moss peat. Water Res. 2000, 34, 735–742. [Google Scholar] [CrossRef]
- Ho, Y.; McKay, G. Pseudo-second order model for sorption processes. Process Biochem. 1999, 34, 451–465. [Google Scholar] [CrossRef]
- Fan, L.; Luo, C.; Sun, M.; Li, X.; Qiu, H. Highly selective adsorption of lead ions by water-dispersible magnetic chitosan/graphene oxide composites. Colloids Surf. B 2013, 103, 523–529. [Google Scholar] [CrossRef]
Isothermal Adsorption Model | Parameter | NH3·H2O-Zeolite 4A | KH792-Zeolite 4A |
---|---|---|---|
Langmuir model | Qmax (mg/g) | 53.55 | 42.93 |
KL (L/mg) | 0.003 | 0.0014 | |
RL | 0.625 | 0.78 | |
R2 | 0.9997 | 0.9993 | |
Freundlich model | Kf (mg/g) | 25.36 | 0.29 |
R2 | 0.9958 | 0.9977 |
Pseudo First-Order Dynamics | Pseudo Second-Order Dynamics | |||||
---|---|---|---|---|---|---|
Qe (mg/g) | K1 | R2 | Qe (mg/g) | K2 | R2 | |
NH3·H2O-zeolite 4A | 1.79 | 0.27 | 0.4194 | 1.97 | 0.21 | 0.9063 |
KH792-zeolite 4A | 1.74 | 0.28 | 0.4293 | 1.87 | 0.16 | 0.9617 |
ΔH° (kJ/mol) | ΔS° (kJ/mol·K) | ΔG° (kJ/mol) | |||
---|---|---|---|---|---|
25 °C | 35 °C | 45 °C | |||
NH3·H2O-zeolite 4A | −89.22 | 0.13 | −127.96 | −130.56 | −133.16 |
KH792-zeolite 4A | −93.08 | 0.17 | −143.74 | −147.14 | −150.54 |
Sample | Adsorption Condition | Maximum Adsorption Capacity (mg/g) | References |
---|---|---|---|
Thiol- and hydroxyl-containing bifunctional vermiculite | pH 4 and dosage 2 g/L | 8.57 | [47] |
Adsorption columns using activated carbon and zeolite | pH from 0 to 7 and dosage 1 g/L | 5.5 | [48] |
Opal-palygorskite clay zeolite 4A | pH 3 and dosage 1 g/L | 41.99 | [49] |
13X zeolite | pH from 5 to 6 and dosage 100 g/L | 16.35 | [50] |
KH792-zeolite 4A | pH 6 and 5 g/L | 42.93 | This work |
NH3·H2O-zeolite 4A | pH 6 and 5 g/L | 53.55 | This work |
Washing Time (h) | |||||
---|---|---|---|---|---|
6 | 12 | 24 | 36 | 48 | |
Adding NH3·H2O-zeolite 4A | 0.013 | 0.112 | 0.157 | 0.142 | 0.170 |
No adding | 1.065 | 3.355 | 5.76 | 5.74 | 5.82 |
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Gao, M.; Yang, L.; Yang, S.; Jiang, T.; Wu, F.; Nagasaka, T. Simple Aminated Modified Zeolite 4A Synthesized Using Fly Ash and Its Remediation of Mercury Contamination: Characteristics and Mechanism. Sustainability 2022, 14, 15924. https://doi.org/10.3390/su142315924
Gao M, Yang L, Yang S, Jiang T, Wu F, Nagasaka T. Simple Aminated Modified Zeolite 4A Synthesized Using Fly Ash and Its Remediation of Mercury Contamination: Characteristics and Mechanism. Sustainability. 2022; 14(23):15924. https://doi.org/10.3390/su142315924
Chicago/Turabian StyleGao, Mengdan, Liyun Yang, Shuangjian Yang, Tong Jiang, Fei Wu, and Tetsuya Nagasaka. 2022. "Simple Aminated Modified Zeolite 4A Synthesized Using Fly Ash and Its Remediation of Mercury Contamination: Characteristics and Mechanism" Sustainability 14, no. 23: 15924. https://doi.org/10.3390/su142315924