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Cu/UiO-66: a novel nanocatalyst obtained by a microwave-assisted protocol in DMF-free media for the efficient phenol removal via catalytic wet peroxide oxidation
Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2020-08-06 , DOI: 10.1016/j.jece.2020.104332
Luis A. Lozano , Alejandra Devard , María A. Ulla , Juan M. Zamaro

This paper analyzes the microwave-assisted synthesis of the zirconium-based metal-organic framework (MOF) UiO-66 using acetone as a solvent, in replacement of the traditional and toxic N,N-Dimethylformamide (DMF). It also studies the subsequent loading of this MOF with high amounts of dispersed copper species to be used as catalyst in the advanced oxidation of phenol. To this purpose, the structural development of UiO-66 was monitored studying the effect of synthesis variables such as stirring, temperature, treatment time and volume of the mixture. In this way, a high-crystallinity UiO-66 was obtained with high yields (88 %) at short times (6 h) and under mild conditions (80 °C) in a DMF-free media. Subsequently, by studying treatment conditions, a Cu/UiO-66 catalyst supporting high loadings (10 wt. %) of highly dispersed copper species (Cu+/Cu2+) was obtained. This nanocatalyst, which was obtained following sustainability criteria, exhibited a high performance in the catalytic wet peroxide oxidation (CWPO) of phenol, quickly converting all the phenol at 70 °C in the first 5 min and reaching a mineralization (TOC removal) of 88 % and a H2O2 consumption efficiency of 30 % at 120 min. Cu/UiO-66 represents a new nanostructured catalyst based on highly dispersed copper species to be applied in CWPO processes.



中文翻译:

Cu / UiO-66:一种新型纳米催化剂,通过微波辅助方案在不含DMF的介质中通过催化湿式过氧化物氧化有效去除苯酚

本文以丙酮为溶剂,代替了传统的有毒N,N-二甲基甲酰胺(DMF),分析了微波辅助合成锆基金属有机骨架(MOF)UiO-66。它还研究了此MOF的后续负载量,该负载量带有大量分散的铜物质,可在苯酚的高级氧化中用作催化剂。为此,对UiO-66的结构发展进行了监测,研究了诸如搅拌,温度,处理时间和混合物体积等合成变量的影响。以此方式,在无DMF的介质中,在短时间内(6小时)和温和条件(80°C)下以高收率(88%)获得了高结晶度的UiO-66。随后,通过研究处理条件,得到支持高负载量(10重量%)的高度分散的铜物种(Cu)的Cu / UiO-66催化剂获得+ / Cu 2+。遵循可持续性标准获得的这种纳米催化剂在苯酚的催化湿式过氧化物氧化(CWPO)中表现出出色的性能,在前5分钟内于70°C迅速将所有苯酚转化,并达到88的矿化度(去除TOC) %和120分钟的H 2 O 2消耗效率为30%。Cu / UiO-66代表了一种新的基于高度分散的铜物种的纳米结构催化剂,将用于CWPO工艺中。

更新日期:2020-08-06
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