Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue

doi:10.1016/j.cjche.2022.03.010

中国化学工程学报 ›› 2023, Vol. 53 ›› Issue (1): 251-259.DOI: 10.1016/j.cjche.2022.03.010

• Full Length Article • 上一篇下一篇

Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue

Hongwei Guo¹, Linyuan Chen², Xueying Zhang², Huanhao Chen¹, Yan Shao²

1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China;
2. School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, China

收稿日期:2021-10-10 修回日期:2022-02-25 出版日期:2023-01-28 发布日期:2023-04-08
通讯作者: Huanhao Chen,E-mail:h.chen@njtech.edu.cn;Yan Shao,E-mail:y.shao@njtech.edu.cn
基金资助:
It is greatly appreciate the funding support from the Jiangsu Province Dual Creative Phds Program (JSSCBS20210400), and the Jiangsu Specially-Appointed Professors Program.

Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue

Hongwei Guo¹, Linyuan Chen², Xueying Zhang², Huanhao Chen¹, Yan Shao²

1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China;
2. School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, China

Received:2021-10-10 Revised:2022-02-25 Online:2023-01-28 Published:2023-04-08
Contact: Huanhao Chen,E-mail:h.chen@njtech.edu.cn;Yan Shao,E-mail:y.shao@njtech.edu.cn
Supported by:
It is greatly appreciate the funding support from the Jiangsu Province Dual Creative Phds Program (JSSCBS20210400), and the Jiangsu Specially-Appointed Professors Program.

摘要/Abstract

摘要： Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants. Herein, Fe nanocatalysts were encapsulated into silicalite-1 (S-1) zeolite by using a ligand-protected method (with dicyandiamide (DCD) as a organic ligand) under direct hydrothermal synthesis condition. High-resolution transmission electron microscopy (HRTEM) results confirmed the high dispersion of Fe nanocatalysts which were successfully encapsulated within the voids among the primary particles of the S-1 zeolite. The developed S-1 zeolite encapsulated Fe nanocatalyst (Fe@S-1) exhibited significantly improved catalytic activity and reusability in the catalytic degradation process of methylene blue (MB). Specifically, the developed Fe_0.021@S-1 catalyst showed high catalytic degradation activity, giving a high MB degradation efficiency of 100% in 30 min, outperformed the conventional impregnated catalyst (Fe/S-1). Moreover, the Fe@S-1 catalyst afforded an outstanding stability, showing only ca. 7.9% activity loss after five cycling tests, while the Fe/S-1 catalyst presented a significantly activity loss of 50.9% after only three cycles. Notably, the encapsulation strategy enabled a relatively lower Fe loading in the Fe@S-1 catalyst in comparison with that of the Fe/S-1 catalyst, i.e., 0.35% vs. 0.81% (mass). Radical scavenging experiments along with electron spin resonance (ESR) measurements confirmed that the major role of OH in the MB degradation process. Specifically, Fe@S-1 catalyst with high molar ratio of [Fe(DCD)]Cl₃ is beneficial to form Fe complexes/nanoclusters in the voids (which has large pore size of 1–2 nm) among the primary particles of the zeolite, and thus improving the diffusion and accessibility of reactants to Fe active sites, and thus exhibiting a relatively higher degradation efficiency. This work demonstrates that zeolite-encapsulated Fe nanocatalysts present potential applications in the advanced oxidation of wastewater treatment.

关键词: Zeolite, Encapsulation, Fe nanocatalyst, Degradation, Methylene blue

Abstract: Encapsulation of Fe nanoparticles in zeolite is a promising way to significantly improve the catalytic activity and stability of Fe-based catalysts during the degradation process of organic pollutants. Herein, Fe nanocatalysts were encapsulated into silicalite-1 (S-1) zeolite by using a ligand-protected method (with dicyandiamide (DCD) as a organic ligand) under direct hydrothermal synthesis condition. High-resolution transmission electron microscopy (HRTEM) results confirmed the high dispersion of Fe nanocatalysts which were successfully encapsulated within the voids among the primary particles of the S-1 zeolite. The developed S-1 zeolite encapsulated Fe nanocatalyst (Fe@S-1) exhibited significantly improved catalytic activity and reusability in the catalytic degradation process of methylene blue (MB). Specifically, the developed Fe_0.021@S-1 catalyst showed high catalytic degradation activity, giving a high MB degradation efficiency of 100% in 30 min, outperformed the conventional impregnated catalyst (Fe/S-1). Moreover, the Fe@S-1 catalyst afforded an outstanding stability, showing only ca. 7.9% activity loss after five cycling tests, while the Fe/S-1 catalyst presented a significantly activity loss of 50.9% after only three cycles. Notably, the encapsulation strategy enabled a relatively lower Fe loading in the Fe@S-1 catalyst in comparison with that of the Fe/S-1 catalyst, i.e., 0.35% vs. 0.81% (mass). Radical scavenging experiments along with electron spin resonance (ESR) measurements confirmed that the major role of OH in the MB degradation process. Specifically, Fe@S-1 catalyst with high molar ratio of [Fe(DCD)]Cl₃ is beneficial to form Fe complexes/nanoclusters in the voids (which has large pore size of 1–2 nm) among the primary particles of the zeolite, and thus improving the diffusion and accessibility of reactants to Fe active sites, and thus exhibiting a relatively higher degradation efficiency. This work demonstrates that zeolite-encapsulated Fe nanocatalysts present potential applications in the advanced oxidation of wastewater treatment.

Key words: Zeolite, Encapsulation, Fe nanocatalyst, Degradation, Methylene blue

Hongwei Guo, Linyuan Chen, Xueying Zhang, Huanhao Chen, Yan Shao. Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue[J]. 中国化学工程学报, 2023, 53(1): 251-259.

Hongwei Guo, Linyuan Chen, Xueying Zhang, Huanhao Chen, Yan Shao. Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue[J]. Chinese Journal of Chemical Engineering, 2023, 53(1): 251-259.

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Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue

Silicalite-1 zeolite encapsulated Fe nanocatalyst for Fenton-like degradation of methylene blue

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