Reduction of Fe(II)EDTA-NO with palladium based catalysts
REN Xiaocong1, HU Zirui2, ZHANG Guangxu2
(1.Department of Biological and Chemical Engineering, Zhixing College of HuBei University, Wuhan 430070, China; 2.School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China)
摘要Fe(Ⅱ)EDTA络合脱硝法对一氧化氮(NO)具有良好的吸收效果,是脱硝技术重点研究方向,但Fe(Ⅱ)EDTA-NO络合液再生困难限制了它的发展.为达到Fe(II)EDTA络合液循环使用的目的,以阴离子交换树脂IRA900为载体,通过浸渍法负载钯前驱体,经硼氢化钠还原后制备出了Pd/IRA900催化剂.通过X射线衍射、X射线光电子能谱图、透射电子显微镜、热重分析等表征表明,Pd/IRA900催化剂中钯纳米微团的平均粒径为2.14 nm,Pd0含量为84%(质量分数),对还原Fe(II)EDTA-NO有着良好的催化活性.搭建一套可持续运转的流化床试验装置,评价结果如下:在气相的条件为总流量200 L ·h-1、NO含量为0.07%(体积分数)、含氧量10%,络合液再生条件为初始浓度0.05 mol ·L-1、温度60 ℃、pH=5、液气比6的最佳工艺条件下,可以维持脱硝率90%以上稳定运行300 min.
Abstract:Fe(II)EDTA complexation denitrification method has a good absorption effect on nitric oxide (NO) and is an important research direction in denitrification technology. However, the difficulty in regenerating Fe(II)EDTA-NO complexation solution limits its development. To achieve the goal of recycling Fe(II)EDTA complex solution, Pd/IRA900 catalyst was prepared using anion exchange resin IRA900 as a carrier, and palladium precursor was loaded by impregnation method, followed by reduction with sodium borohydride. X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric analysis showed that the average particle size of palladium nanoclusters in Pd/IRA900 catalyst was 2.14 nm with the Pd0 content of 84% (mass fraction) and the Pd/IRA900 catalyst exhibited good catalytic activity for reducing Fe (II) EDTA-NO. A sustainable fluidized bed testing device was builded, and the evaluation results were as follows: under the optimal process conditions of total gas flow rate of 200 L·h-1, NO concentration of 0.07% (volume fraction), oxygen content of 10%, initial complex solution concentration of 0.05 mol/L, temperature of 60 ℃, pH=5 and liquid gas ratio of 6, the denitrification rate could be maintained above 90% for stable operation over 300 min.