Fe负载UiO-66协同非均相类Fenton氧化降解废气苯的研究

张婷婷; 周长松; 周梦长; 吴昊; 张振; 杨宏旻

doi:10.19906/j.cnki.JFCT.2021013

Fe负载UiO-66协同非均相类Fenton氧化降解废气苯的研究

doi: 10.19906/j.cnki.JFCT.2021013

南京师范大学能源与机械工程学院，江苏南京 210023

基金项目: 国家自然科学基金（51906114），江苏省自然科学基金（BK20180731）和中国博士后科学基金（2018T110523）资助

详细信息

通讯作者:
E-mail: cszhou@njnu.edu.cn

中图分类号: X511
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出版历程
- 收稿日期: 2020-09-29
- 修回日期: 2020-11-09
- 刊出日期: 2021-02-08

Study on the synergistic heterogeneous Fenton oxidation degradation of benzene containing waste gas using Fe doped UiO-66

School of Energy & Mechanical Engineering, Nanjing Normal University, Nanjing 210023, China

Funds: The project was supported by the National Natural Science Foundation of China (51906114), National Science Foundation of Jiangsu Province (BK20180731), China Postdoctoral Science Foundation Project (2018T110523)

More Information

Corresponding author: E-mail: cszhou@njnu.edu.cn

摘要

摘要: 采用水热合成法制备了不同掺杂比例Fe负载UiO-66，并借助XRD、SEM、XPS等分析测试手段对催化剂物理化学特性进行分析，通过自制非均相类Fenton体系装置探究不同Fe负载量、H₂O₂浓度、空塔速率、反应温度等条件下对废气苯的氧化降解效率影响。结果表明，不同Fe负载量的UiO-66均具有较高的结晶度，呈不规则球状；在非均相类Fenton氧化降解苯实验中，30%的Fe负载UiO-66具有最高的苯脱除效率。EPR结果显示，Fe负载量的增大促进·OH的产生，在一定程度上促进苯的氧化降解。过高的反应温度导致H₂O₂不稳定，非均相类Fenton氧化降解苯的效率随温度的升高先增大后降低。
- 催化剂 /
- 苯 /
- 非均相类Fenton /
- 金属有机骨架 /
- 挥发性有机污染物
Abstract: The UiO-66 catalysts with different doping ratio of Fe were prepared by hydrothermal synthesis method in this study. The physicochemical properties of the catalysts were characterized by means of XRD, SEM and XPS. The benzene removal efficiency of the catalysts was investigated using a bench-scaled heterogeneous Fenton-like system device. The effects of Fe loading amount, H₂O₂concentration, superficial velocity and reaction temperature on benzene removal efficiency were studied. The results showed that the Fe doped UiO-66 was irregularly spherical and of high crystallinity. The highest benzene removal efficiency was obtained at 93% over the catalyst with 30% Fe loading. The EPR results proved that increasing Fe loading on UiO-66 evidently promoted the production of ·OH radicals, which promoted the degradation of benzene to a certain extent. The benzene removal efficiency decreased with the rise of temperature at higher range because H₂O₂ was unstable at high temperature.
- catalyst /
- benzene /
- heterogeneous Fenton /
- metal organic framework /
- volatile organic compounds

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图 1 实验装置流程示意图

Figure 1 Schematic diagram of the experimental apparatus

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图 2 不同Fe负载量的Fe/UiO-66催化剂的XRD谱图

Figure 2 XRD patterns of the Fe/UiO-66 catalysts with different Fe loadings

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图 3 不同Fe负载量的Fe/UiO-66催化剂的SEM照片

Figure 3 SEM images of the Fe/UiO-66 catalysts with different Fe loadings

(a)：10% Fe/UiO-66；(b)：20% Fe/UiO-66; (c)：30% Fe/UiO-66；(d)：40% Fe/UiO-66

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图 4 不同Fe负载量的Fe/UiO-66的XPS谱图

Figure 4 XPS patterns of the Fe/UiO-66 catalysts with different Fe loadings

(a)：survey scans；(b)：Fe 2p spectra；(c)：O 1s spectra

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图 5 Fe负载量对苯氧化降解效率的影响

Figure 5 Effect of Fe loading on benzene removal efficiency

(reaction conditions: the initial concentration is 600 mg/m³, temperature is 130 ℃, H₂O₂ concentration is 1 mol/L)

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图 6 H₂O₂浓度对不同Fe掺杂量Fe/UiO-66催化剂氧化降解苯的影响

Figure 6 Effect of H₂O₂ concentration on benzene removal by four Fe/UiO-66 catalysts with different Fe loadings (reaction conditions: the initial concentration is 600 mg/m³, temperature is 130 ℃)

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图 7 空塔速率对30% Fe/UiO-66非均相类Fenton氧化降解苯的影响

Figure 7 Effect of superficial velocity on benzene removal by 30% Fe/UiO-66 heterogeneous Fenton reaction (reaction conditions: the initial concentration is 600 mg/m³, temperature is 130 ℃, H₂O₂ concentration is 1 mol/L)

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图 8 反应温度对30% Fe/UiO-66非均相Fenton氧化降解苯的影响

Figure 8 Effect of reaction temperature on benzene removal by 30% Fe/UiO-66 heterogeneous Fenton reaction (reaction conditions: the initial concentration is 600 mg/m³, the concentration of H₂O₂ is 1 mol/L)

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图 9 10% Fe/UiO-66、20% Fe/UiO-66、30% Fe/UiO-66和40% Fe/UiO-66类Fenton反应过程的EPR波谱强度

Figure 9 EPR spectrum intensity of 10% Fe/UiO-66, 20% Fe/UiO-66, 30% Fe/UiO-66 and 40% Fe/Ui O-66 Fenton reaction processes

reaction conditions: H₂O₂ concentration is 1 mol/L, DMPO concentration is 5 mmol/L and reaction measurement time is 15 min

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图 10 30% Fe/UiO-66催化剂的稳定性

Figure 10 Stability test of the 30% Fe/UiO-66 catalyst

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表 1 催化剂的比表面积及孔容

Table 1 Surface area and pore volume of the catalysts with different Fe loadings

Sample S_BET/(m²·g⁻¹) Pore volume/(cm³·g⁻¹)

10% Fe/UiO-66 1007.0 0.346
20% Fe/UiO-66 1021.8 0.333
30% Fe/UiO-66 1210.5 0.428
40% Fe/UiO-66 1169.7 0.440

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