铁柱撑蒙脱石表面介导的Fe(Ⅱ)还原体系对邻硝基苯酚的高效去除

卢鹏澄; 魏燕富; 吴宏海; 张璇; 陈静

doi:10.6054/j.jscnun.2021056

铁柱撑蒙脱石表面介导的Fe(Ⅱ)还原体系对邻硝基苯酚的高效去除

doi: 10.6054/j.jscnun.2021056

华南师范大学环境学院，广州 510006

基金项目:

国家自然科学基金项目 42072046

国家自然科学基金项目 41372050

广东省自然科学基金项目 2018B030311021

详细信息

通讯作者:
魏燕富，Email: yanfuwei@m.scnu.edu.cn

中图分类号: X523, O647.3
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- 文章访问数: 281
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- PDF下载量: 22
- 被引次数: 0
出版历程
- 收稿日期: 2021-04-26
- 网络出版日期: 2021-09-03
- 刊出日期: 2021-08-25

The Surface-mediated Fe(Ⅱ) Reduction System of Iron-pillared Montmorillonite for Efficient Removal of 2-Nitrophenol

School of Environment, South China Normal University, Guangzhou 510006, China

摘要

摘要: 通过引入铁氧化物并煅烧处理对蒙脱石进行优化设计，成功合成了铁柱撑蒙脱石复合催化剂(FPMt).采用X射线衍射(XRD)、热重分析(TG)、透射电子显微镜(TEM)、傅里叶变换红外光谱(FT-IR)、N₂吸附-脱附(BET)等分析方法对FPMt样品结构与表面性质进行表征，以邻硝基苯酚(2-NP，22 μmol/L)作为代表性污染物研究FPMt的还原催化活性. 结果表明：与蒙脱石相比，FPMt表面电子传输活性得到明显提高，原因是引入赤铁矿的FPMt吸附位点增多同时酸位减少，从而显著增强材料表面的还原催化活性. 除溶液pH和Fe(Ⅱ)浓度外，催化剂的结构完整性、赤铁矿的结晶度等均为影响催化剂还原活性的重要因素. 最后提出了FPMt表面络合态Fe(Ⅱ)的还原催化活性显著提高的介导机制.
- 铁柱撑蒙脱石 /
- 煅烧 /
- 亚铁 /
- 还原催化 /
- 邻硝基苯酚(2-NP) /
- 赤铁矿
Abstract: Iron-pillared montmorillonite composite catalyst (FPMt) was successfully synthesized by optimizing the design of montmorillonite through the introduction of iron oxides and the calcination treatment. The structural and surface properties of FPMt samples were characterized with X-ray diffraction (XRD), thermogravimetric analysis (TG), TEM, FT-IR, N₂ adsorption and desorption isotherms, and 2-Nitrophenol (2-NP, 22 μmol/L) was used as a representative pollutant to identify the reduction catalytic activity of FPMt. The results showed that, compared to montmorillonite, the surface electron transport activity of FPMt was significantly improved due to the increase of adsorption sites of Fe(Ⅱ) and the corresponding reduction of acid sites on the surface of FPMt, significantly enhancing the reduction catalytic performance of the material. In addition to the solution pH and Fe(Ⅱ) concentration, the structural integrity of the catalyst and the crystallinity of hematite are important factors affecting the catalytic activity. Finally, a mediating mechanism for the significant increase in the reduction catalytic activity of complexed Fe(Ⅱ) on the surface of FPMt was proposed.
- iron-pillared montmorillonite /
- calcination /
- ferrous /
- catalytic reduction /
- 2-Nitrophenol /
- hematite

HTML全文

图 1 铁柱撑蒙脱石样品的XRD图谱

Figure 1. The XRD patterns of different FPMt samples

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图 2 FPMt的TG、DTG、DSC图

Figure 2. The TG, DTG, DSC curves of FPMt

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图 3 Mt和不同煅烧温度下FPMt的红外光谱

Figure 3. The FT-IR spectra of Mt and FPMt samples under different calcination temperatures

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图 4 不同铁柱撑蒙脱石的TEM图

Figure 4. The TEM images of different FPMt samples

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图 5 不同铁柱撑蒙脱石的N₂吸脱附等温线

Figure 5. The N₂ adsorption-desorption isotherms of different FPMt samples

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图 6 不同FPMt样品对2-NP的还原去除曲线

Figure 6. The reductive removal curves of 2-NP by different FPMt samples

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图 7 不同FPMt样品对2-NP的去除率

Figure 7. The removal rate of 2-NP by different FPMt samples

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图 8 不同FPMt样品对Fe²⁺的去除率

Figure 8. Fe²⁺ remoral rate of different FPMt samples

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图 9 不同Py-FPMt样品的红外光谱

Figure 9. The FT-IR spectra of different Py-FPMt samples

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表 1 不同FPMt样品的比表面积和孔结构数据

Table 1. The specific surface area and porosity data of different FPMt samples

样品	比表面积/(m²·g^-1)	总孔容积/(cm³·g^-1)	平均孔径/nm
FPMt	126.875 3	0.101 4	5.346 7
FPMt100	112.736 3	0.078 8	4.792 6
FPMt200	138.538 7	0.112 8	4.462 9
FPMt300	144.010 8	0.123 0	4.344 1
FPMt400	165.693 8	0.136 9	4.198 7
FPMt500	155.070 2	0.142 1	4.380 7

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表 2 不同FPMt样品的阳离子交换量

Table 2. The cation exchange capacity of different FPMt samples

催化剂	Na⁺交换量/(mol·(100 g)^-1)
Mt原样	99
FPMt	92
FPMt100	68
FPMt200	61
FPMt300	55
FPMt400	31
FPMt500	22
注：Na⁺交换量以每100 g材料吸附Na⁺的物质的量(mol)计算.

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