Torrellas Silvia A, Escudero Gabriel O, Rodriguez Araceli R, Rodriguez Juan G
a Catalysis and Separation Process Group (CyPS), Chemical Engineering Department, Faculty of Chemistry , Complutense University of Madrid , Madrid , Spain.
J Environ Sci Health A Tox Hazard Subst Environ Eng. 2015;50(4):372-7. doi: 10.1080/10934529.2015.987529.
The effect of acid treatments with HCl and HNO3 on the surface area and surface chemistry of three granular activated carbons was studied. These supports were characterized and the hydrochloric acid treatment leads to the best activated carbon support (AC2-C). The catalytic behavior of Pt, Ru and Fe (1 wt.%) supported on granular activated carbon treated with HCl was tested in the phenylamine continuous catalytic wet air oxidation in a three-phase, high-pressure catalytic reactor over a range of reaction temperatures 130-170ºC and total pressure of 1.0-3.0 MPa at LHSV = 0.4-1 h(-1), whereas the phenylamine concentration range and the catalyst loading were 5-16 mol.m(-3) and 0.5-1.5 g, respectively. Activity as well as conversion varied as a function of the metal, the catalyst preparation method and operation conditions. Higher activities were obtained with Pt incorporated on hydrochloric acid -treated activated carbon by the ion exchange method. In steady state, approximately 98% phenylamine conversion, 77% of TOC and 94% of COD removal, was recorded at 150ºC, 11 mol m(-3) of phenylamine concentration and 1.5 g of catalyst, and the selectivity to non-organic compounds was 78%. Several reaction intermediaries were detected. A Langmuir-Hinshelwood model gave an excellent fit of the kinetic data of phenylamine continuous catalytic wet air oxidation over the catalysts of this work.
研究了用盐酸和硝酸进行酸处理对三种颗粒活性炭的表面积和表面化学性质的影响。对这些载体进行了表征，盐酸处理得到了最佳的活性炭载体（AC2-C）。在三相高压催化反应器中，在130 - 170℃的反应温度范围和1.0 - 3.0 MPa的总压力下，液时空速为0.4 - 1 h⁻¹，对负载在经盐酸处理的颗粒活性炭上的Pt、Ru和Fe（1 wt.%）的催化行为进行了测试，苯胺浓度范围和催化剂负载量分别为5 - 16 mol·m⁻³和0.5 - 1.5 g。活性和转化率随金属、催化剂制备方法和操作条件而变化。通过离子交换法将Pt负载在盐酸处理的活性炭上可获得更高的活性。在稳态下，在150℃、苯胺浓度为11 mol m⁻³和催化剂为1.5 g时，记录到苯胺转化率约为98%，总有机碳去除率为77%，化学需氧量去除率为94%，对非有机化合物的选择性为78%。检测到了几种反应中间体。Langmuir-Hinshelwood模型对这项工作中催化剂上苯胺连续催化湿式空气氧化的动力学数据拟合良好。
