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Copper-based ternary hydrotalcite as a catalyst for hydroxylation of phenolic compounds
Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2021-09-20 , DOI: 10.1016/j.jece.2021.106390
Rongrong Dai 1 , Baogui Liu 2 , Yan Zhang 1 , Jacob Nedergaard Pedersen 1 , Xiaowen Zhang 1, 3 , Mingdong Dong 4 , Zheng Guo 1
Affiliation  

Hydrotalcites with different cations were synthesized by co-precipitation method and characterized using different techniques. The catalytic activity of the hydrotalcites was studied using hydroxylation of phenol by H2O2 as a model reaction. The CuNiAl ternary hydrotalcite was found to be the best catalyst in this work; and the effects of reaction temperature, ratio of substrate:catalyst, H2O2 concentration, solvent and pH value of the medium were investigated. The results showed that under optimal reaction conditions, the conversion of phenol can reach up to 62.8%, with catechol and hydroquinone as the main products. The substrate scope was expanded to other phenol-derivatives, such as m-cresol and 3-ethylphenol. A plausible reaction mechanism was proposed based on the control reactions and XPS analysis. The CuNiAl hydrotalcite shows high toxicity (the 48 h LC50 value of CuNiAl hydrotalcite was 2.12 mg/L) in the acute toxicity tests of Daphnia magna. However, after simple filtration of the solid catalyst, the 48 h LC50 value of the remaining solution was increased to 83.46 mg/L. In all, the as-synthesized CuNiAl35 hydrotalcite offers a novel biodegradation pathway for in situ treatment of phenol-contaminated water or other phenolic pollutions when applied together with dioxygenases for further degradation of resulting catechols or hydroquinones.



中文翻译:

铜基三元水滑石作为酚类化合物羟基化的催化剂

不同阳离子的水滑石是通过共沉淀法合成的,并使用不同的技术进行表征。使用H 2 O 2对苯酚的羟基化作为模型反应来研究水滑石的催化活性。CuNiAl三元水滑石被发现是这项工作中最好的催化剂;以及反应温度、底物与催化剂的比例、H 2 O 2 的影响考察了培养基的浓度、溶剂和pH值。结果表明,在最佳反应条件下,苯酚的转化率可达62.8%,主要产物为邻苯二酚和对苯二酚。底物范围扩大到其他苯酚衍生物,如间甲酚和 3-乙基苯酚。基于控制反应和XPS分析提出了一个合理的反应机理。CuNiAl水滑石在大型水的急性毒性试验中表现出高毒性(CuNiAl水滑石的48 h LC 50值为2.12 mg/L)。然而,在对固体催化剂进行简单过滤后,48 h LC 50剩余溶液的值增加到 83.46 mg/L。总之,当与双加氧酶一起应用时,合成的 CuNiAl35 水滑石为苯酚污染的水或其他酚类污染的原位处理提供了一种新的生物降解途径,以进一步降解所得的儿茶酚或对苯二酚。

更新日期:2021-09-24
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