【作者】 张翼；

【导师】 赵朝成；

【作者基本信息】 中国石油大学 ， 环境工程， 2009， 硕士

【摘要】 本文针对石化企业停工检修时产生的含硫恶臭污染特点及污染现状,以低浓度硫化氢气体为研究对象,采用吸收氧化技术和活性炭吸附催化氧化技术对实验室模拟含硫恶臭气体治理进行了初步研究。通过实验考察了影响吸收氧化法脱除H₂S效率的因素,对吸收氧化机理及动力学过程进行了研究。利用硝酸铜对颗粒活性炭浸渍改性,考察了影响改性活性炭吸附H₂S效率的因素,研究了吸附催化氧化机理及其动力学过程。探讨了吸收-吸附联合工艺应用于中试实验处理硫化氢恶臭气体的可行性。吸收氧化法实验结果表明:在H₂S进气浓度不超过6000mg·m^-3,进气流量0.4L·min^-1,吸收液中碳酸钠浓度50g·L^-1,催化剂浓度0.3g·L^-1,吸收氧化温度50℃的条件下,H₂S去除效率能在较长时间内保持在99%以上。吸收液采用空气曝气法再生。吸收氧化机理分析表明吸收氧化的最终产物主要为单质硫。研究H₂S的浓度对吸收速率的影响,得到了吸收速率方程式。经动力学分析,H₂S与液相中Na2CO3的反应为慢速反应,反应在液膜和液相主体中进行。在相关实验条件下,吸附催化氧化法实验结果表明:与未改性活性炭相比,浸渍硝酸铜的改性活性炭对H₂S的吸附能力显著增强,在2%附近为最佳浸渍量。改性活性炭的床层高度和穿透时间成线性关系。随着H₂S入口浓度的提高,床层穿透时间下降较快。较低的空间速度下吸附性能较好。在25-75℃范围内吸附温度变化对床层的穿透时间影响不大。表面pH测定结果表明,SO2或H₂SO4可能是改性活性炭吸附H₂S的主要产物。XRD分析结果显示,浸渍改性后铜主要以CuO的形式负载在活性炭表面上;吸附穿透后,硫主要以CuSO4·5H2O的形式固定下来。元素分析结果表明,浸渍2%硝酸铜的改性活性炭吸附H₂S穿透后的元素硫含量由吸附前的0.2%增至16.72%,说明浸渍硝酸铜改性可以显著提高活性炭的硫容量。动力学分析结果认为硝酸铜改性活性炭吸附气体中低含量H₂S的等温线为Frendlich型,并且得到了吸附速率方程式。根??试实验要求,设计出了相应的??吸收塔和固定床吸附器。更多还原

【Abstract】 According to the sulf-odor pollution characteristic and present situation generated from the examining and repairing downtime in petrochemical enterprise, the study target was H₂S gas in low concentration. The preliminary study on the treatment of lab simulated sulf-odor with absorption oxidization technology and adsorption-catalytic oxidation by activated carbon was carried out. The absorption oxidation influencing factors were investigated in the laboratory experiment. The absorption oxidation mechanism and dynamics process also have been discussed in this paper. The granular activated carbon was modified by impregnating Cu（NO₃）₂. The factors which influenced the modified activated carbon adsorbing H₂S were investigated in the laboratory experiment. The adsorption-catalytic oxidation mechanism and dynamics process also have been discussed. We discuss the feasibility which the joint technology of absorption and adsorption are applied to handle the hydrogen sulfide odor in field experiment.The results of absorption oxidization experiment showed that when sodium carbonate concentration maintained at a level of 50g·L-1, catalyst concentration at a level of 0.3g·L-1, and the absorption oxidation temperature maintained at 50℃, the removal efficiency of H₂S could maintain above 99% for a long time within the concentration of 6000 mg·m^-3. The absorption solution could be regenerated through aeration. The analysis of absorption oxidization principle indicated that the main absorption oxidation product was sulfur. Through researching how the concentration of hydrogen sulfide affected the absorption rate, I got an absorption reaction equation. The analysis of dynamics indicated that the reaction was a slow reaction. The reaction took place in the liquid film and the main body of liquid phase.In the relevant experimental conditions, the results of adsorption-catalytic oxidation experiment showed that when the activated carbon modified by impregnating Cu（NO3）2, the adsorption capacity of H₂S increased markedly compared with the unmodified activated carbon. The volume of the best impregnation was nearby 2%. The bed height and the penetration time of the modified activated carbon had a linear relationship. The penetration time declined rapidly when the entrance concentration of H₂S increased. The adsorption capability was much better under the lower space velocity. The change of temperature had little influence on the penetration time of activated carbon in the range of 25-75℃. The result of surface pH measuration showed that sulfur dioxide and sulphuric acid might be the main products. XRD analysis showed that copper was loaded in the form of CuO on the activated carbon after the activated carbon modified by impregnating Cu（NO₃）₂. When the activated carbon was penetrated, sulfur mainly fixed in the form of CuSO₄·5H₂O. When the activated carbon modified by impregnating Cu（NO₃）₂ was penetrated, the elemental sulfur content on the activated carbon rose from 0.2% to 16.72%. It indicated modified with Cu（NO₃）₂ could significantly enhance the sulfur capacity of the activated carbon. The result of dynamics analysis indicated that the adsorption isotherm of actived carbon modified with Cu（NO₃）₂ accorded with Frendlich’equation. I also got the adsorption rate equation.According to the requirements of the field experiment, the padding absorber and fixed bed adsorber have been designed.更多还原