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钯/氨修饰 MIL-101(Cr)促进的氢加速类芬顿体系对 4-氯苯酚的破坏作用。

Destruction of 4-chlorophenol by the hydrogen-accelerated catalytic Fenton system enhanced by Pd/NH-MIL-101(Cr).

机构信息

Jiangsu Key Laboratory of Environmental Science and Engineering, Institute of Environmental Protection Application Technology, School of Environmental Science and Engineering, Tianping College of Suzhou University of Science and Technology, Suzhou University of Science and Technology, Suzhou, People's Republic of China.

Suzhou Mengli Environmental Technology Co., Ltd., Suzhou, People's Republic of China.

出版信息

Environ Technol. 2022 Apr;43(10):1561-1572. doi: 10.1080/09593330.2020.1841831. Epub 2020 Nov 26.

DOI:10.1080/09593330.2020.1841831
PMID:33115346
Abstract

4-chlorophenol (4-CP) could be rapidly mineralized by using Fenton reaction. However, massive iron sludge will be generated because of the excessive consumption of iron salt and poor recycling of Fe back to Fe. In this paper, by introducing hydrogen gas and solid catalyst Pd/NH-MIL-101(Cr) to classic Fenton reactor, the novel system named MHACF-NH-MIL-101(Cr) was constructed. Much less Fe was needed in this system because the hydrogen could significantly accelerate the regeneration of Fe. The catalyst improved the utilization of H. The degradation reaction of 4-CP could be driven by using only trace amount of Fe. It could be rapidly degraded by the hydroxyl radical detected by the 4-Hydroxy-benzoicacid which is the oxidative product of benzoic acid and hydroxyl radical. The effects of dosage of ferrous salt, HO and catalyst, H flow, Pd content, and initial pH of and concentration of 4-CP aqueous solution were investigated. The robustness and morphology changes of this catalytic material were also systematically analysed. By clarifying the role of this solid MOFs material in this hydrogen-mediated Fenton reaction system, it will provide a new direction for the research and development of advanced oxidation processes with high efficiency and low sludge generation in future.

摘要

4-氯苯酚(4-CP)可以通过芬顿反应快速矿化。然而,由于铁盐的大量消耗和 Fe 无法有效回收利用,会产生大量的铁污泥。在本文中,通过向经典芬顿反应器中引入氢气和固体催化剂 Pd/NH-MIL-101(Cr),构建了一种名为 MHACF-NH-MIL-101(Cr)的新型系统。由于氢气可以显著加速 Fe 的再生,该系统所需的 Fe 量要少得多。催化剂提高了 H 的利用率。仅需痕量的 Fe 就可以驱动 4-CP 的降解反应。通过检测到的 4-羟基苯甲酸(苯甲酸和羟基自由基的氧化产物)来检测羟基自由基,可以快速降解 4-CP。考察了亚铁盐、HO 和催化剂、H 流量、Pd 含量、初始 pH 值以及 4-CP 水溶液浓度等因素对反应的影响。还系统地分析了这种催化材料的稳定性和形貌变化。通过阐明这种固体 MOFs 材料在这种氢介导的芬顿反应体系中的作用,为今后高效、低污泥生成的高级氧化工艺的研究和开发提供了新的方向。

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