Resource Recycling of Red Soil to Synthesize Fe2O3/FAU-type Zeolite Composite Material for Heavy Metal Removal
Summary
This article presents a novel and convenient route to synthesize Fe2O3/faujasite (FAU)-type zeolite composite material from red soil. The detailed synthesis parameters have been finely tuned. The obtained composite material can be used for efficient heavy metal-contaminated water remediation, indicating its potential applications in environmental engineering.
Abstract
Heavy metal-polluted water is of great concern to human health and the eco-environment. In situ water remediation techniques enabled by highly efficient adsorption materials are of great importance in these circumstances. Among all the materials used in water remediation, iron-based nanomaterials and porous materials are of great interest, benefiting from their rich redox reactivity and adsorption function. Here, we developed a facile protocol to directly convert the widely spread red soil in south China to fabricate the Fe2O3/faujasite (FAU)-type zeolite composite material.
The detailed synthesis procedure and synthesis parameters, such as reaction temperature, reaction time, and the Si/Al ratio in the raw materials, have been carefully tuned. The as-synthesized composite materials show good adsorption capacity for typical heavy metal(loid) ions. With 0.001 g/mL Fe2O3/FAU-type zeolite composite material added to different heavy metal(loid)-polluted aqueous solutions (single type of heavy metal(loid) concentration: 1,000 mg/L [ppm]), the adsorption capacity was shown to be 172, 45, 170, 40, 429, 693, 94, and 133 mg/g for Cu (II), Cr (III), Cr (VI), As (III), Cd (II), Pb (II), Zn (II), and Ni (II) removal, respectively, which can be further expanded for heavy metal-polluted water and soil remediation.
Introduction
Heavy metal(loid)s from anthropogenic and natural activities are ubiquitous in the air, water, and soil environment1. They are of high mobility and toxicity, posing a potential health risk to human beings by direct contact or via food chain transportation2. Water is vital for the life of human beings since it is the feedstock of every family. Restoring water health is crucial. Therefore, it is of great importance to decrease the mobility and bioavailability of toxic heavy metal(loid)s in water. To maintain good health in water, water remediation materials, such as biochar, iron-based materials, and zeolite, play an essential role in immobilizing or removing heavy metal(loid)s from aqueous environments3,4,5.
Zeolites are highly crystalline materials with unique pores and channels in their crystal structures. They are composed of TO4 tetrahedra (T is the central atom, usually Si, Al, or P) connected by shared O atoms. The negative surface charge and exchangeable ions in the pores make it a popular adsorbent for ion capture, which has been extensively used in heavy metal-polluted water and soil remediation. Benefiting from their structures, the remediation mechanisms involved in contaminant removal by zeolites mainly include chemical bonding6, surface electrostatic interaction7, and ion exchange8.
Faujasite (FAU)-type zeolite has relatively large pores, with a maximum pore diameter of 11.24 Å. It shows high efficiency and broad applications for contaminant removal9,10. In recent years, extensive research has devoted to developing green and low-cost routines for zeolite synthesis, such as using industrial solid wastes11 as raw material to provide silicon and aluminium sources, or adopting directing agent-free recipes12. The reported alternative industrial solid wastes that can be silicon and aluminum sources include coal gangue13, fly ash11, waste molecular sieves14, mining and metallurgical wastes15, engineering-abandoned soil8, and agricultural soil6, etc.
Herein, red soil, an abundant and easily obtained silicon and aluminum-rich material, was adopted as the raw material, and a facile green chemistry approach was developed for Fe2O3/FAU-type zeolite composite material synthesis (Figure 1). The detailed synthesis parameters have been finely tuned. The as-synthesized material shows high immobilization capacity for heavy metal-contaminated water remediation. The present study should be instructive for related researchers who are interested in this area to use soil as a raw material for eco-material synthesis.
Protocol
Representative Results
Discussion
Zeolite is typically an aluminosilicate material. In theory, materials that are rich in silicate and aluminate can be chosen as raw materials for zeolite synthesis. The Si/Al ratio of the raw material must be similar to that of the selected type of zeolite to minimize the usage of additional silicon/aluminum sources6,8,16. The Si/Al ratio of FAU-type zeolite is 1.2, and the Si/Al ratio of red soil is 1.3. Therefore, red soil is …
Divulgazioni
The authors have nothing to disclose.
Acknowledgements
This work was financially supported by the Natural Science Funds for Distinguished Young Scholar of Guangdong Province, China, No. 2020B151502094; National Natural Science Foundation of China, No. 21777045 and 22106064; Foundation of Shenzhen Science, Technology and Innovation Commission, China, JCYJ20200109141625078; 2019 youth innovation project of Guangdong universities and colleges, China, No. 2019KQNCX133 and a special fund for the science and technology innovation strategy of Guangdong Province (PDJH2021C0033). This work was sponsored by the Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (No. ZDSYS20200421111401738), Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control (2017B030301012), and State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control. In particular, we acknowledge the technical support from the SUSTech Core Research Facilities.
Materials
| Chemicals | |||
| Cadmium nitrate tetrahydrate | Shanghai Aladdin Bio-Chem Technology Co., LTD | C102676 | AR, 99%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Chromium(III) nitrate nonahydrate | Shanghai Aladdin Bio-Chem Technology Co., LTD | C116446 | AR, 99%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Copper sulfate pentahydrate | Shanghai Aladdin Bio-Chem Technology Co., LTD | C112396 | AR, 99%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Lead nitrate | Shanghai Aladdin Bio-Chem Technology Co., LTD | L112118 | AR, 99%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Nickel nitrate hexahydrate | Shanghai Aladdin Bio-Chem Technology Co., LTD | N108891 | AR, 98%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Nitric acid | Shanghai Aladdin Bio-Chem Technology Co., LTD | N116238 | AR, 69.2%. Used as solvent in ICP-MS test. |
| Potassium dichromate | Shanghai Aladdin Bio-Chem Technology Co., LTD | P112163 | AR, 99.8%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Silicon dioxide | Shanghai Aladdin Bio-Chem Technology Co., LTD | S116482 | AR, 99%. For synthesis of zeolite. |
| Sodium (meta)arsenite | Sigma-aldrich | S7400-100G | AR, 90%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Sodium hydroxide | Shanghai Aladdin Bio-Chem Technology Co., LTD | S111502 | Pellets. For the synthesis of zeolite. |
| Zinc nitrate hexahydrate | Shanghai Aladdin Bio-Chem Technology Co., LTD | Z111703 | AR, 99%. Make 1,000 ppm stock solution for the test of adsorption performance of zeolite. |
| Equipment | |||
| Air-dry oven | Shanghai Yiheng Technology Instrument Co.,LTD. | DHG-9075A | Used for hydrothermal crystallization and drying of sample |
| Analytical balance | Sartorius Scientific Instruments Co.LTD | BSA224S-CW | Used for weighing samples |
| Centrifuge tubes | Nantong Supin Experimental Equipment Co., LTD | ||
| High speed centrifuge | Hunan Xiang Yi Laboratory Instrument Development Co.,LTD | H1850 | Used for separation of solid and liquid samples |
| Multipoint magnetic stirrer | IKA Equipment Co.,LTD. | RT15 | Used for stirring samples |
| Oscillator | Changzhou Guohua Electric Appliances Co.,LTD. | SHA-B | For uniform mixing of samples |
| Syringe-driven filter | Tianjin Jinteng Experimental Equipment Co.,LTD. | 0.22 μm. For filtration. | |
| Softwares | |||
| JADE 6.5 | Materials Data& (MDI) | ||
| Mercury | Cambridge Crystallographic Data Centre (CCDC) | ||
| Materials Studio | Accelrys Software Inc. | ||
| Websites | |||
| Database of Zeolite Structures: http://www.iza-structure.org/databases/ | |||
| ICSD: https://icsd.products.fiz-karlsruhe.de/en |
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