硅酸盐学报

纳米片形MFI-Fe分子筛活化H₂O₂降解酸性红G

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许飞亚 ¹ , 姬亚军 ² , 杨鸿辉 ³ , 李清飞 ² , 张宗文 ¹ , 郭沛音 ¹ , 刘明华 ²

硅酸盐学报 | 研究论文 2024,52(11): 3492-3501

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硅酸盐学报 |研究论文 2024 , 52 (11) : 3492 -3501

纳米片形MFI-Fe分子筛活化H₂O₂降解酸性红G

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许飞亚¹, 姬亚军², 杨鸿辉³, 李清飞², 张宗文¹, 郭沛音¹, 刘明华²

作者信息

^1．信阳师范大学分析测试中心，河南信阳 464000

^2．信阳师范大学地理科学学院/河南省水土环境污染协同防治重点实验室，河南信阳 464000

^3．西安交通大学化学学院，西安 710049

通讯作者:

姬亚军（1990—），男，博士，副教授。

作者简介:

许飞亚（1990—），女，硕士，实验师。

Degradation of Acidic Red G by H₂O₂ Activated with Nanosheet MFI-Fe Zeolite

Feiya XU¹, Yajun JI², Honghui YANG³, Qingfei LI², Zongwen ZHANG¹, Peiyin GUO¹, Minghua LIU²

Affiliations

^1.Analysis & Testing Center, Xinyang Normal University, Xinyang 464000, Henan, China

^2.Henan Key Laboratory for Synergistic Prevention of Water and Soil Environmental Pollution/School of Geographic Sciences, Xinyang Normal University, Xinyang 464000, Henan, China

^3.School of Chemistry, Xi'an Jiaotong University, Xi'an 710049, China

Corresponding Author:

JI Yajun (1990-), male, Ph.D., Associate Professor. E-mail: jiyajun928@163.com

XU Feiya (1990-), female, Master, Lab Master. E-mail: Xufy1104@163.com

出版时间: 2024-11-20 doi: 10.14062/j.issn.0454-5648.20230960

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摘要

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传统类芬顿催化剂在酸性条件下易溶出Fe导致活性下降。通过合成纳米片形MFI-Fe分子筛，将Fe镶嵌在分子筛骨架中，抑制Fe溶出，使其保持稳定的催化活性。结果表明：MFI-Fe通过活化H₂O₂产生HO•使酸性红G（ARG）降解。在pH=3、25 ℃、0.40 g/L MFI-Fe、20 mmol/L H₂O₂、180 min条件下，ARG（20 mg/L）的去除率达到约98.40%。溶液中NO₃^-、Cl^-、SO₄^2-共存离子对ARG的去除无影响，腐殖酸（HA）会轻微抑制ARG的降解。HCO₃^-会使溶液pH值升高，并消耗HO•导致ARG的去除率显著下降。反复使用5次MFI-Fe，Fe浸出量均小于0.42 mg/L，ARG的去除率保持在87.64%以上。

关键词

MFI分子筛 / 类芬顿反应 / 酸性红G / 降解

Abstract

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Introduction

The easy dissolution of Fe under acidic conditions results in the decreased activity of traditional Fenton-like catalysts. It was reported that the encapsulated or framework stabilized Fe-based materials showed excellent stability. Zeolite is a crystalline silicate/aluminosilicate with a stable framework structure, high specific surface area, uniform microporous and mesoporous structure, good acid-base resistance property. These characteristics make it a promising carrier or main material for Fenton-like catalysts. Therefore, a Fe-doped nanosheet MFI (MFI-Fe) zeolite was synthesized in this study. The Fe sites was embedded in the framework of MFI-Fe zeolite to inhibit the dissolution of Fe under acidic conditions, which could improve the performance of MFI-Fe zeolite for activating H₂O₂ towards acidic red G (ARG) degradation in water.

Methods

With the assistance of diquaternary ammonium-type structural directing agents, the solid products were obtained through hydrothermal reactions (160 ℃, 5 d) using tetraethyl orthosilicate and ferric chloride as the main raw materials. Then, MFI-Fe zeolite was obtained by calcining the solid products in air at 550 ℃ for 3 h. X-ray diffraction spectroscopy (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), fourier transform infrared spectroscopy (FTIR), N₂ adsorption-desorption and X-ray photoelectron spectroscopy (XPS) were applied to determine the physicochemical properties of MFI-Fe zeolite. The prepared MFI-Fe zeolite was applied to active H₂O₂ for ARG degradation. The effects of catalyst dosage, H₂O₂ dosage, solution pH value, reaction temperature, ARG concentration and coexisting ions on the degradation of ARG were studied. The concentration of ARG in the water was determined by an ultraviolet and visible (UV-Vis) spectrophotometer.

Results and discussion

According to the XRD and FTIR results, the prepared MFI-Fe zeolite exhibited the characteristic peaks of MFI zeolite, and there were not impurity peaks of silicon oxide or iron oxide, indicating that both silicon and iron entered into the framework of MFI zeolite. The XPS spectra of MFI-Fe zeolite exhibited peaks of Fe 2p_3/2 and Fe 2p_1/2 at 711.8 eV and 725 eV, respectively. They were very close to the binding energies of the 2p_3/2 and 2p_1/2 peaks of Fe₂O₃. Moreover, there was no Fe²⁺ peak (approximately 708 eV) in MFI-Fe zeolite. These results indicated that Fe in MFI-Fe zeolite existed in the form of +3 valence and was directly connected to O. The SEM images showed that MFI-Fe zeolite was composed of many nanosheets. Si and Fe were uniformly distributed in the crystals. According to the N₂ adsorption and desorption results, the specific surface area and external surface area of MFI-Fe zeolite reached to 343.71 m²·g^-1 and 176.78 m²·g^-1, respectively. The average pore size of MFI-Fe zeolite reached 4.19 nm. These structural characteristics endowed MFI-Fe zeolite with excellent catalytic activity. The catalytic experiment results showed that ARG could only be rapidly removed when both H₂O₂ and MFI-Fe zeolite existed. The reaction mechanism results indicated that HO•was generated by the activating of H₂O₂ with MFI-Fe zeolite, leading to the degradation of ARG. In solution having pH values of 3-9, the removal rates of ARG gradually decreased with the increase of pH values. It can be explained that a lower pH value conduced to the activation of H₂O₂, thereby accelerating the degradation of ARG. Under the optimum conditions (initial pH=3, 25 ℃, MFI-Fe 0.40 g/L, H₂O₂ 20 mmol/L), the removal rate of ARG (20 mg/L) reached to 98.40% within 180 min. The coexistence of NO₃^-, Cl^-, and SO₄^2- in the solution had not effect on the removal of ARG. The degradation of ARG was slightly inhibited by humic acid (HA). The removal rate of ARG was significantly slowed down with the coexistence of HCO₃^-. It can be explained that the pH value of the solution would increase and partial HO• would be consumed when HCO₃^- is added into the reaction system. After reuse for 5 times, the concentrations of leached Fe were less than 0.42 mg/L, and the removal rates of ARG exceeded 87.64%.

Conclusions

A nanosheet MFI-Fe zeolite was synthesized and applied to active H₂O₂ for ARG degradation. When the pH value of the solution was between 3 and 9, the removal rates of ARG gradually decreased with the increase of the solution pH values. The reaction rate reached to the maximum (0.023 min^-1) at a pH value of 3. Under the optimal conditions (pH=3, 25 ℃, 0.40 g/L MFI-Fe and 20 mmol/L H₂O₂), the removal rate of ARG (20 mg/L) reached approximately 98.40% within 180 min. The coexistence of NO₃^-, Cl^-, and SO₄^2- ions in the solution had not effect on the removal of ARG, while the degradation of ARG was slightly inhibited by humic acid (HA). The removal rate of ARG decreased significantly with the coexistence of HCO₃^-. After reuse for 5 times, the concentrations of leached Fe were less than 0.42 mg/L, and the removal rates of ARG exceeded 87.64%.

Key words

MFI zeolite / fenton-like reaction / acidic red G / degradation

引用本文

许飞亚, 姬亚军, 杨鸿辉, 李清飞, 张宗文, 郭沛音, 刘明华. 纳米片形MFI-Fe分子筛活化H₂O₂降解酸性红G. 硅酸盐学报, 2024 , 52 (11) : 3492 -3501 . DOI: 10.14062/j.issn.0454-5648.20230960

Feiya XU, Yajun JI, Honghui YANG, Qingfei LI, Zongwen ZHANG, Peiyin GUO, Minghua LIU. Degradation of Acidic Red G by H₂O₂ Activated with Nanosheet MFI-Fe Zeolite[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (11) : 3492 -3501 . DOI: 10.14062/j.issn.0454-5648.20230960

基金

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国家自然科学基金(41671476)
河南省科技攻关项目(24210 2320078)
河南省高等学校重点科研项目(21A610010)
信阳师范大学“南湖学者奖励计划”青年项目
河南省水土环境污染协同防治重点实验室开放基金(KLSPWSEP-A05)
信阳师范大学青年科研基金项目(2024-QN-043)

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2024年第52卷第11期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230960

接收时间：2023-12-10
首发时间：2026-10-22
出版时间：2024-11-20

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收稿日期：2023-12-10
修回日期：2024-01-01

基金

国家自然科学基金(41671476)

河南省科技攻关项目(24210 2320078)

河南省高等学校重点科研项目(21A610010)

信阳师范大学“南湖学者奖励计划”青年项目

河南省水土环境污染协同防治重点实验室开放基金(KLSPWSEP-A05)

信阳师范大学青年科研基金项目(2024-QN-043)

作者信息

^1．信阳师范大学分析测试中心，河南信阳 464000

^2．信阳师范大学地理科学学院/河南省水土环境污染协同防治重点实验室，河南信阳 464000

^3．西安交通大学化学学院，西安 710049

通讯作者:

姬亚军（1990—），男，博士，副教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230960

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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