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^III back to Fe^II. In this paper, by introducing hydrogen gas and solid catalyst Pd/NH₂-MIL-101(Cr) to classic Fenton reactor, the novel system named MHACF-NH₂-MIL-101(Cr) was constructed. Much less Fe^II was needed in this system because the hydrogen could significantly accelerate the regeneration of Fe^II. The catalyst improved the utilization of H₂. The degradation reaction of 4-CP could be driven by using only trace amount of Fe^II. 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, H₂O₂ and catalyst, H₂ 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。但是，由于铁盐消耗过多以及^三价铁回收到^二价铁的不良，会产生大量的铁泥。本文通过将氢气和固体催化剂Pd/NH ₂ -MIL-101(Cr)引入经典Fenton反应器，构建了MHACF-NH ₂ -MIL-101(Cr)的新型体系。在这个系统中需要更少的^二价铁，因为氢气可以显着加速^二价铁的再生。该催化剂提高了H ₂的利用率。仅使用微量的 Fe ^{II即可驱动 4-CP 的降解反应}. 苯甲酸与羟基自由基的氧化产物4-羟基苯甲酸检测到的羟基自由基能迅速降解。研究了亚铁盐、H ₂ O ₂和催化剂的用量、H ₂流量、Pd含量以及4-CP水溶液初始pH和浓度的影响。还系统地分析了这种催化材料的稳健性和形态变化。通过阐明这种固体MOFs材料在这种氢介导的Fenton反应体系中的作用，将为未来高效、低产泥量的高级氧化工艺的研发提供新的方向。