混合价态铁基金属有机框架催化过氧乙酸高效降解对硝基苯酚

doi:10.13475/j.fzxb.20210902908

纺织学报 ›› 2022, Vol. 43 ›› Issue (11): 133-140.doi: 10.13475/j.fzxb.20210902908

混合价态铁基金属有机框架催化过氧乙酸高效降解对硝基苯酚

胡倩¹^,², 杨涛语¹, 朱斐超³, 吕汪洋³^,⁴, 吴明华¹^,³, 余德游¹^,²^,⁴()

1.浙江理工大学生态染整技术教育部工程研究中心, 浙江杭州 310018
2.浙江理工大学桐乡研究院, 浙江嘉兴 314500
3.浙江理工大学先进纺织材料与制备技术教育部重点实验室, 浙江杭州 310018
4.浙江理工大学材料科学与工程学院, 浙江杭州 310018

收稿日期:2021-09-09 修回日期:2022-03-15 出版日期:2022-11-15 发布日期:2022-12-26
通讯作者: 余德游
作者简介:胡倩(1991—),女,博士生。主要研究方向为印染废水处理及再生利用。
基金资助:
国家自然科学基金项目(22106141);中国博士后科学基金项目(2022M712827);浙江理工大学桐乡研究院博士后基金资助项目(TYY202103)

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. 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 Published:2022-11-15 Online:2022-12-26
Contact: YU Deyou

摘要/Abstract

摘要：

为提升铁基金属有机框架(Fe-MOFs)对印染废水深度处理的效能,采用原位掺杂溶剂热技术制备了混合Fe(Ⅱ)/Fe(Ⅲ)价态MIL-53(Fe)(MV-MIL-53(Fe))催化剂。借助X射线粉末衍射仪、场发射扫描电镜、氮气吸附仪和吡啶吸附红外光谱仪等对MV-MIL-53(Fe)晶体结构、微观形貌、孔结构和表面酸位等本征结构进行了测试分析。选取对硝基苯酚(4-NP)作为印染废水模型污染物,以过氧乙酸(PAA)为氧源,研究了MV-MIL-53(Fe)催化PAA降解4-NP的性能和关键活性物种。结果表明:Fe(Ⅱ)的引入提高了MIL-53(Fe)表面Lewis酸位密度,为PAA催化活化提供了更丰富更高效的活性位点;MV-MIL-53(Fe)/PAA体系对4-NP的降解速率常数高达0.052 1 min^-1,分别是MV-MIL-53(Fe)/H₂O₂、MIL-53(Fe)/PAA和MIL-53(Fe)/H₂O₂体系的2.05、1.45和6.68倍,且MV-MIL-53(Fe)重复循环使用5次后仍保持良好的结构稳定性和催化降解性能;羟基自由基(·OH)是MV-MIL-53(Fe)催化PAA快速降解4-NP的关键活性物质。

关键词: 铁基金属有机框架, 过氧乙酸, 催化降解, 对硝基苯酚, 印染废水

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

中图分类号:

O643.32

胡倩, 杨涛语, 朱斐超, 吕汪洋, 吴明华, 余德游. 混合价态铁基金属有机框架催化过氧乙酸高效降解对硝基苯酚[J]. 纺织学报, 2022, 43(11): 133-140.

HU Qian, YANG Taoyu, ZHU Feichao, LÜ Wangyang, WU Minghua, YU Deyou. Peracetic acid activation for efficient degradation of p-nitrophenol by mixed-valence iron-based metal-organic framework[J]. Journal of Textile Research, 2022, 43(11): 133-140.

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参考文献 25

[1]	章耀鹏, 沈忱思, 徐晨烨, 等. 纺织工业典型污染物治理技术回顾[J]. 纺织学报, 2021, 45(8): 24-33.
	ZHANG Yaopeng, SHEN Chensi, XU Chenye, et al. Review on treatment technology for typical pollutants in textile industry[J]. Journal of Textile Research, 2021, 45(8): 24-33.
[2]	LIN X Q, KONG W M, LIN X. Degradation of high-concentration p-nitrophenol by Fenton oxidation[J]. Water Science & Technology, 2020, 81(10): 2260-2269.
[3]	D'ALMEIDA S R, BUORO R M. Determination of p-nitrophenol in synthetic textile wastewater samples using a graphene oxide/palladium nanoparticles modified carbon paste electrode[J]. Electroanalysis, 2021, 33: 1623-1632. doi: 10.1002/elan.202060539
[4]	王海人, 石兴阳, 徐育, 等. 废铁屑处理含酚废水的新方法及其机理研究[J]. 环境科学与技术, 2010, 33(12): 309-311.
	WANG Hairen, SHI Xingyang, XU Yu, et al. New method of scrap iron dealing with p-nitrophenol simulated wastewater and the research of its mechanism[J]. Environmental Science & Technology, 2010, 33(12): 309-311.
[5]	杨明, 刘琪, 孙健, 等. 印染废水深度处理研究及应用进展[J]. 净水技术, 2020, 39(10): 109-115.
	YANG Ming, LIU Qi, SUN Jian, et al. Research and application progress of advanced treatment of dyeing wastewater[J]. Water Purification Technology, 2020, 39(10): 109-115.
[6]	PEREIRA A, RODRIGUES F, PAULINO A, et al. Recent advances on composite hydrogels designed for the remediation of dye-contaminated water and wastewater: a review[J]. Journal of Cleaner Production, 2021, 284: 124703. doi: 10.1016/j.jclepro.2020.124703
[7]	EPSZTEIN R, DUCHANOIS R, RITT C, et al. Towards single-species selectivity of membranes with subnanometre pores[J]. Nature Nanotechnology, 2020, 15(6): 426-436. doi: 10.1038/s41565-020-0713-6 pmid: 32533116
[8]	胡承志, 刘会娟, 曲久辉. 电化学水处理技术研究进展[J]. 环境工程学报, 2018, 12(3): 677-696.
	HU Chengzhi, LIU Huijuan, QU Jiuhui. Research progress of electrochemical technologies for water treatment[J]. Chinese Journal of Environmetal Engineering, 2018, 12(3): 677-696.
[9]	HODGES B, CATES E, KIM J. Challenges and prospects of advanced oxidation water treatment processes using catalytic nanomaterials[J]. Nature Nanotechnology, 2018, 13(8): 642-650. doi: 10.1038/s41565-018-0216-x pmid: 30082806
[10]	YANG Z, QIAN J, YU A, et al. Singlet oxygen mediated iron-based Fenton-like catalysis under nanoconfinement[J]. Proceedings of the National Academy of Sciences of the United States of America, 2019, 116(14): 6659-6664. doi: 10.1073/pnas.1819382116 pmid: 30872470
[11]	ZHOU P, REN W, NIE G, et al. Fast and long-lasting iron(Ⅲ) reduction by boron toward green and accelerated Fenton chemistry[J]. Angewandte Chemie International Edition, 2020, 59(38): 16517-16526. doi: 10.1002/anie.202007046
[12]	SUN M, CHU C, GENG F, et al. Reinventing Fenton chemistry: iron oxychloride nanosheet for pH-insensitive H₂O₂ cctivation[J]. Environmental Science & Technology Letters, 2018, 5(3): 186-191.
[13]	ZHAO H, QIAN L, GUAN X, et al. Continuous bulk FeCuC aerogel with ultradispersed metal nanoparticles: an efficient 3D heterogeneous electro-Fenton cathode over a wide range of pH 3-9[J]. Environmental Science & Technology, 2016, 50(10): 5225-5233. doi: 10.1021/acs.est.6b00265
[14]	XIA Q, WANG H, HUANG B, et al. State-of-the-art advances and challenges of iron-based metal organic frameworks from attractive features, synthesis to multifunctional applications[J]. Small, 2018, 15(2): 1803088.
[15]	YU D, WU M, HU Q, et al. Iron-based metal-organic frameworks as novel platforms for catalytic ozonation of organic pollutant: efficiency and mechanism[J]. Journal of Hazardous Materials, 2019, 367: 456-464. doi: S0304-3894(18)31257-3 pmid: 30611038
[16]	WU Q, YANG H, KANG L, et al. Fe-based metal-organic frameworks as Fenton-like catalysts for highly efficient degradation of tetracycline hydrochloride over a wide pH range: acceleration of Fe(Ⅱ)/Fe(Ⅲ) cycle under visible light irradiation[J]. Applied Catalysis B: Environmental, 2020, 263: 1-6.
[17]	GAO C, CHEN S, QUAN X, et al. Enhanced Fenton-like catalysis by iron-based metal organic frameworks for degradation of organic pollutants[J]. Journal of Catalysis, 2017, 356: 125-132. doi: 10.1016/j.jcat.2017.09.015
[18]	TANG J, WANG J. Metal-organic framework with coordinatively unsaturated sites as efficient Fenton-like catalyst for enhanced degradation of sulfamethazine[J]. Environmental Science & Technology, 2018, 52(9): 5367-5377. doi: 10.1021/acs.est.8b00092
[19]	AO X, ELORANTA J, HUANG C, et al. Peracetic acid-based advanced oxidation processes for decontamination and disinfection of water: a review[J]. Water Reseach, 2021, 188: 1-6.
[20]	EBRAHIM A, BANDOSZ T. Ce(III) doped Zr-based MOFs as excellent NO₂ adsorbents at ambient condi-tions[J]. ACS Applied Materials Interfaces, 2013, 5(21): 10565-10573. doi: 10.1021/am402305u
[21]	GAO C, SU Y, QUAN X, et al. Electronic modulation of iron-bearing heterogeneous catalysts to accelerate Fe(III)/Fe(II) redox cycle for highly efficient Fenton-like catalysis[J]. Applied Catalysis B: Environmental, 2020, 276: 1-8.
[22]	THOMMES M, KANEKO K, NEIMARK ALEXANDER V, et al. Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report)[J]. Pure and Applied Chemistry, 2015, 87(9/10): 1051-1069. doi: 10.1515/pac-2014-1117
[23]	LECLERC H, VIMONT A, LAVALLEY J, et al. Infrared study of the influence of reducible iron(Ⅲ) metal sites on the adsorption of CO, CO₂, propane, propene and propyne in the mesoporous metal-organic framework MIL-100[J]. Physical Chemistry Chemical Physics, 2011, 13(24): 11748-11756. doi: 10.1039/c1cp20502a
[24]	BING J, HU C, ZHANG L. Enhanced mineralization of pharmaceuticals by surface oxidation over mesoporous γ-Ti-Al₂O₃ suspension with ozone[J]. Applied Catalysis B: Environmental, 2017, 202: 118-126. doi: 10.1016/j.apcatb.2016.09.019
[25]	WANG J, WANG Z, CHENG Y, et al. Molybdenum disulfide (MoS₂): a novel activator of peracetic acid for the degradation of sulfonamide antibiotics[J]. Water Research, 2021, 201: 1-5.

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样品名称	酸位强度	酸位密度/(mmol·g^-1)
样品名称	酸位强度	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

混合价态铁基金属有机框架催化过氧乙酸高效降解对硝基苯酚

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

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