溶剂热法合成用于高效光催化燃油脱氮的TiO<sub>2</sub>@MIL-101(Cr)复合材料

LU Yi; LIANG Ruo-wen; YAN Gui-yang; LIANG Zhi-yu; HU Wei-neng; XIA Yu-zhou; HUANG Ren-kun

doi:10.1016/S1872-5813(21)60170-6

溶剂热法合成用于高效光催化燃油脱氮的TiO₂@MIL-101(Cr)复合材料

doi: 10.1016/S1872-5813(21)60170-6

卢沂^{1, 2,},
梁若雯^{1, 2, 3},
颜桂炀¹,
梁志喻^{1, 3},
胡未能²,
夏宇宙¹,
黄仁昆^{1, 2, 3, ,}

1.
宁德师范学院福建省绿色能源与环境催化高校重点实验室福建宁德，352100
2.
福州大学能源与环境光催化国家重点实验室，福建福州，350002
3.
宁德师范学院福建省特色生物化工材料重点实验室福建宁德，352100

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中图分类号: O643.32
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出版历程
- 收稿日期: 2021-08-04
- 修回日期: 2021-09-23
- 网络出版日期: 2021-10-25
- 刊出日期: 2022-04-26

Solvothermal synthesis of TiO₂@MIL-101(Cr) for efficient photocatalytic fuel denitrification

LU Yi^{1, 2
,},
LIANG Ruo-wen^{1, 2, 3},
YAN Gui-yang¹,
LIANG Zhi-yu^{1, 3},
HU Wei-neng²,
XIA Yu-zhou¹,
HUANG Ren-kun^{1, 2, 3
, ,}

1.
Province University Key Laboratory of Green Energy and Environment Catalysis, Ningde Normal University, Ningde 352100, China
2.
State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, China
3.
Fujian Provincial Key Laboratory of Featured Materials in Biochemical Industry, Ningde Normal University, Ningde 352100, China

Funds: The project was supported by Program for Innovative Research Team in Science and Technology in Fujian Province University, Natural Science Foundation of Fujian Province (2019J05121), Research Project of Ningde Normal University (2019T03) and the Training Program Foundation for Distinguished Young Scholar by Fujian Province.

More Information

Author Bio:
957832459@qq.com

Corresponding author: Tel: +86-593-2965018; E-mail: t1432@ndnu.edu.cn

摘要

摘要: 溶剂热合成技术是一种有效合成复合材料的技术。在本研究中，通过溶剂热法制备了不同比例复合的TiO₂@MIL-101(Cr)复合材料。并利用这些材料进行可见光光催化燃油脱氮（吡啶）。对所得催化剂采用XRD、FT-IR、SEM、TEM、BET和DRS进行表征。通过活性实验结果可以得到，20%TiO₂@MIL-101(Cr)具有良好的催化活性，在可见光光照4 h后，对吡啶的脱除率高达70%。最后，通过对HPLC-MS数据分析，得到一个光催化燃油脱氮的可能机理。
- 光催化 /
- 燃油 /
- 脱氮 /
- MIL-101(Cr) /
- TiO₂
Abstract: Solvothermal synthesis technique is an effective method to create composite materials. In this paper, a series of TiO₂@MIL-101(Cr) were prepared by the solvothermal method for photocatalytic denitrification of pyridine in fuel under visible light irradiation. The products were characterized by XRD, FT-IR, SEM, TEM, BET, DRS and ESR. The result shows that 20%TiO₂@MIL-101(Cr) has high catalytic activity, the pyridine removal efficiency reaches values as high as 70% after irradiation for 240 min. Finally, we obtained the possible mechanism of photocatalytic denitrification according to the HPLC-MS spectrometry results analysis.
- photocatalytic /
- fuel /
- denitrification /
- MIL-101(Cr) /
- TiO₂

HTML全文

FIG. 1467. FIG. 1467.

FIG. 1467.

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Figure 1 XRD patterns of TiO₂@MIL-101(Cr), MIL-101(Cr) and TiO₂

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Figure 2 SEM images of (a) MIL-101(Cr), (b) 5%MIL-101(Cr), (c) 10%MIL-101(Cr) (d) 20%MIL-101(Cr) and (e) 50%MIL-101(Cr)

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Figure 3 (a) TEM of 20%TiO₂@MIL-101(Cr), ((b), (c)) HRTEM of 20%TiO₂@MIL-101(Cr), (d) C, (e) Cr, (f) Ti

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Figure 4 (a) FT-IR spectra of MIL-101(Cr) and (b) comparison FT-IR spectra of MIL-101(Cr) and 20%TiO₂@MIL-101(Cr)

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Figure 5 N₂ adsorption/desorption isotherms curves of MIL-101(Cr) and x%TiO₂@MIL-101(Cr) (x=5, 10, 20, 50)

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Figure 6 (a) UV-vis DRS spectra of TiO₂ and x%TiO₂@MIL-101(Cr) composites and (b) (Ahν)² vs hν of (a )MIL-101 (Cr), (b) 20%TiO₂@MIL-101 (Cr) and (c) 50%TiO₂@MIL-101 (Cr)

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Figure 7 (a) Photocatalytic denitrogenation of pyridine over MIL-101(Cr), TiO₂ and 20%TiO₂@MIL-101(Cr) under visible light and black, (b) photocatalytic denitrogenation of pyridine at different content of TiO₂

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Figure 8 (a) Transient photocurrent responses of MIL-101(Cr) and 20%TiO₂@MIL-101(Cr), (b) Nyquist impedance plots of MIL-101(Cr) and 20%TiO₂@MIL-101(Cr)

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Figure 9 High-performance liquid chromatography profiles of pyridine after different irradiation times: (a) 0 h and (b) 4 h

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Figure 10 Electron spin response spectra of various radical adducts

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Figure 11 Possible denitrogenation pathway of pyridine

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Table 1 BET surface Area, pore volume of TiO₂@MIL-101(Cr) composites

Sample	BTE surface area/(m²·g⁻¹)	Pore volume/(cm³·g⁻¹)
MIL-101(Cr)	3341.1767	1.63
5%TiO₂@MIL-101(Cr)	2855.3102	1.49
10%TiO₂@MIL-101(Cr)	2585.1894	1.37
20%TiO₂@MIL-101(Cr)	2325.2452	1.23
50%TiO₂@MIL-101(Cr)	1742.2449	0.99

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