Journal of Textile Research ›› 2022, Vol. 43 ›› Issue (11): 133-140.doi: 10.13475/j.fzxb.20210902908

• Dyeing and Finishing & Chemicals • Previous Articles     Next Articles

Peracetic acid activation for efficient degradation of p-nitrophenol by mixed-valence iron-based metal-organic framework

HU Qian1,2, YANG Taoyu1, ZHU Feichao3, LÜ Wangyang3,4, WU Minghua1,3, YU Deyou1,2,4()   

  1. 1. Engineering Research Center for Eco-Dyeing and Finishing of Textiles, Ministry of Education, Zhejiang Sci-Tech University, Hangzhou, Zhejiang 310018, China
    2. Tongxiang Research Institute, Zhejiang Sci-Tech University, Jiaxing, Zhejiang 314500, China
    3. Key Laboratory of Advanced Textile Materials & Manufacturing Technology, Ministry of Education, Zhejiang Sci-Tech University, Hangzhou, Zhejiang 310018, China
    4. School of Materials Science & Engineering, Zhejiang Sci-Tech University, Hangzhou, Zhejiang 310018, China
  • Received:2021-09-09 Revised:2022-03-15 Online:2022-11-15 Published:2022-12-26
  • Contact: YU Deyou E-mail:yudeyou92@zstu.edu.cn

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Abstract:

In order to improve the advanced treatment efficiency of iron-based metal-organic frame-works (Fe-MOFs) for printing and dyeing wastewater, mixed-valence MIL-53(Fe) (MV-MIL-53(Fe)) containing Fe(Ⅱ) and Fe(Ⅲ) was prepared by an in-situ doping solvothermal approach. The MV-MIL-53(Fe) was systematically characterized with X-ray diffraction, scanning electron microscopy, nitrogen adsorption equipment, and pyridine chemisorbed infrared spectroscopy. p-nitrophenol and peracetic acid (PAA) were selected as the model target and green oxidant respectively to study the degradation activity and major active species of MV-MIL-53(Fe). The results show that Fe(Ⅱ) dopant increased the Lewis acidity of MIL-53(Fe), thus offering more active sites for PAA activation. The 4-NP degradation kinetic rate constant of MV-MIL-53(Fe)/PAA system could reach to 0.052 1 min-1, which was 2.05, 1.45, and 6.68 times higher than MV-MIL-53(Fe)/H2O2, MIL-53(Fe)/PAA, and MIL-53(Fe)/H2O2 counterparts, respectively. After successive cycling for five runs, the MV-MIL-53(Fe) still exhibited good structure stability and catalysis activity for 4-NP degradation using PAA. Hydroxyl radicals were verified as the main reactive species converting from PAA for the rapid degradation of 4-NP.

Key words: iron-based metal-organic framework, peracetic acid, catalytic degradation, p-nitrophenol, dyeing and printing wastewater

CLC Number: 

  • O643.32

Fig.1

XRD patterns of MV-MIL-53(Fe) and MIL-53(Fe) catalysts"

Fig.2

Molecular structure and element composition of MV-MIL-53(Fe) and MIL-53(Fe) catalysts. (a) FT-IR spectra; (b) High-resolution Fe 2p XPS spectra"

Fig.3

Morphology and porous structure of MV-MIL-53(Fe) and MIL-53(Fe) catalysts. (a) FE-SEM image; (b) N2 adsorption-desorption curves"

Tab.1

Lewis acidity of prepared MV-MIL-53(Fe) and MIL-53(Fe) catalysts"

样品名称 酸位强度 酸位密度/(mmol·g-1)
细分 总计
MIL-53(Fe) 弱酸 0.48 2.59
中酸 0.82
强酸 1.29
MV-MIL-53(Fe) 弱酸 1.00 3.49
中酸 1.64
强酸 0.85

Fig.4

Comparisons of PAA or H2O2 activation for 4-NP degradation by MV-MIL-53(Fe) and MIL-53(Fe) catalysts. (a) Degradation curves of 4-NP concentration with time; (b) k values of 4-NP degradation in different systems"

Fig.5

Recyclability and stability of MV-MIL-53(Fe). (a) 4-NP degradation curves over five times cycles; (b) XRD pattern of spent MV-MIL-53(Fe); (c) FE-SEM image of spent MV-MIL-53(Fe)(×3 000)"

Fig.6

Identification of major reactive species for 4-NP degradation in MV-MIL-53(Fe)/PAA system. (a) Effect of radical scavengers on 4-NP degradation ; (b) EPR spectra"

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