Quintanilla A, Fraile A F, Casas J A, Rodríguez J J
Area de Ingeniería Química, Facultad de Ciencias, Universidad Autónoma de Madrid, Campus de Cantoblanco, 28049 Madrid, Spain.
J Hazard Mater. 2007 Jul 31;146(3):582-8. doi: 10.1016/j.jhazmat.2007.04.060. Epub 2007 Apr 20.
Catalytic wet peroxide oxidation (CWPO) of phenol with a homemade Fe/activated carbon (Fe/AC) catalyst has been studied in a stainless steel fixed-bed reactor at different operating conditions (T=23-100 degrees C, P(T)=1-8atm, W=0-2.5g, and tau=20-320g(CAT)h/g(Phenol)). The results show that, thanks to the incorporation of Fe on the activated carbon, phenol conversion improved dramatically, reaching a 90% at 65 degrees C, 2atm, and 40g(CAT)h/g(Phenol). However, TOC conversion values remain fairly low, (around 5% at 40g(CAT)h/g(Phenol)), and no improvement was obtained with the inclusion of Fe. The presence of Fe seems to promote the nondesirable coupling reactions that take place in CWPO of phenol due to the condensation of the ring intermediates (the primary phenol oxidation products). These condensation products are quite refractory to CWPO at the conditions employed. Taking advantage of the high phenol conversions in CWPO and the high phenol mineralization in CWAO, along with the good stability of the Fe/AC catalyst, a CWPO-CWAO sequential treatment has been successfully performed by using a fixed-bed and trickle-bed reactor in series. A CWPO treatment at ambient conditions followed by a CWAO treatment at mild conditions (100 degrees C and 8atm) is presented as high efficiency process for the decontamination of phenolic wastewaters.
在不锈钢固定床反应器中,研究了以自制的铁/活性炭(Fe/AC)催化剂对苯酚进行催化湿式过氧化物氧化(CWPO)的过程,考察了不同操作条件(T = 23 - 100℃,P(T) = 1 - 8atm,W = 0 - 2.5g,τ = 20 - 320g(CAT)h/g(Phenol))的影响。结果表明,由于在活性炭上负载了铁,苯酚转化率显著提高,在65℃、2atm和40g(CAT)h/g(Phenol)的条件下达到了90%。然而,总有机碳(TOC)转化率仍然相当低(在40g(CAT)h/g(Phenol)时约为5%),并且负载铁后并未得到改善。铁的存在似乎促进了苯酚CWPO过程中由于环状中间体(苯酚初级氧化产物)的缩合而发生的不良偶联反应。这些缩合产物在所用条件下对CWPO相当难降解。利用CWPO中高的苯酚转化率、催化湿式空气氧化(CWAO)中高的苯酚矿化率以及Fe/AC催化剂的良好稳定性,通过串联使用固定床和滴流床反应器成功进行了CWPO - CWAO顺序处理。提出了在环境条件下进行CWPO处理,随后在温和条件(100℃和8atm)下进行CWAO处理,作为一种高效的含酚废水净化工艺。