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流化床芬顿法中硝基苯氧化及铁结晶的动力学

Kinetics of nitrobenzene oxidation and iron crystallization in fluidized-bed Fenton process.

作者信息

Anotai Jin, Sakulkittimasak Pasootah, Boonrattanakij Nonglak, Lu Ming-Chun

机构信息

Department of Environmental Engineering, Faculty of Engineering, National Center of Excellence for Environmental and Hazardous Waste Management, King Mongkut's University of Technology Thonburi, Bangkok, Thailand.

出版信息

J Hazard Mater. 2009 Jun 15;165(1-3):874-80. doi: 10.1016/j.jhazmat.2008.10.062. Epub 2008 Nov 1.

Abstract

This research investigated the nitrobenzene oxidation and iron removal by fluidized-bed Fenton process using metal oxide as the carriers. It was found that the removal efficiency of nitrobenzene was not affected in the presence of metal oxide. However, metal oxide could retard the degradation rate of nitrobenzene with Fenton process due to ferrous adsorption/complexation onto its surface leaving insufficient free Fe(2+) to catalyze the decomposition of H(2)O(2). Nonetheless, as the free Fe(2+) was sufficient, nitrobenzene was oxidized at the same rate as that by the conventional Fenton process. Fenton's reagent and nitrobenzene concentrations have an impact on nitrobenzene oxidation rate. The empirical kinetic equation for nitrobenzene oxidation by the fluidized-bed Fenton process under the conditions of 0.667-5mM of Fe(2+), 10-50mM of H(2)O(2), 5-12.5mM of nitrobenzene, 76.9 g/l of metal oxide, and pH 2.8+/-0.2, can be described as: [see formula text] Considering on iron removal performance, it was found that the fluidized-bed Fenton process could remove 30-65% of iron via iron crystallization onto the carriers' surface which could lead to a significant reduction in ferric hydroxide sludge production. H(2)O(2) played an important role in iron crystallization and once it was exhausted, the re-dissolution of iron occurred. In addition, it was found that the metal oxide could be repeatedly used up to 5 cycles without any significant deterioration in its surface activity. Hence, it implies that the metal oxide can be used successfully in the fluidized-bed Fenton process operated under a continuous mode.

摘要

本研究考察了以金属氧化物为载体的流化床芬顿工艺对硝基苯的氧化及铁的去除效果。研究发现,金属氧化物的存在不影响硝基苯的去除效率。然而,由于亚铁吸附/络合在金属氧化物表面,导致游离的Fe(2+)不足以催化H(2)O(2)的分解,金属氧化物会减缓芬顿工艺对硝基苯的降解速率。尽管如此,当游离的Fe(2+)充足时,硝基苯的氧化速率与传统芬顿工艺相同。芬顿试剂和硝基苯浓度对硝基苯氧化速率有影响。在Fe(2+)浓度为0.667 - 5mM、H(2)O(2)浓度为10 - 50mM、硝基苯浓度为5 - 12.5mM、金属氧化物浓度为76.9 g/l、pH为2.8±0.2的条件下,流化床芬顿工艺氧化硝基苯的经验动力学方程可描述为:[见公式文本] 考虑到铁的去除性能,发现流化床芬顿工艺可通过铁在载体表面结晶去除30 - 65%的铁,这可显著减少氢氧化铁污泥的产生。H(2)O(2)在铁结晶过程中起重要作用,一旦耗尽,铁会重新溶解。此外,发现金属氧化物可重复使用多达5个循环,其表面活性无明显下降。因此,这意味着金属氧化物可成功用于连续运行模式的流化床芬顿工艺。

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