响应面法优化赤泥负载Co催化剂制备及活性评价  

Preparation of Red Mud Loaded Co Catalysts: Optimization Using Response Surface Methodology ( RSM) and Activity Evaluation

作　　者：李华楠[1] 徐冰冰[2] 齐飞[1,3] 孙德智[1,3] 

机构地区：[1]北京林业大学环境科学与工程学院,北京100083 [2]中国环境科学研究院环境基准与风险评估国家重点实验室,北京100012 [3]北京林业大学北京市水体污染源控制技术重点实验室,北京100083

出　　处：《环境科学》2013年第11期4376-4385,共10页Environmental Science

基　　金：国家自然科学基金项目(51108030;41273137);北京市自然科学基金项目(8132033);高等学校博士学科点专项科研基金项目(20100014120001);中国博士后科学基金项目(201104060;2012M520006)

摘　　要：以催化臭氧氧化去除水中苯扎贝特(bezafibrate,BZF)的处理效果为评价指标,采用Plackett-Burman和响应面(Response Surface Methodology,RSM)法对Co/RM催化剂的制备条件进行优化.结果表明,浸渍质量分数和焙烧温度为催化剂制备的主要影响因素,当浸渍质量分数为4.14%、煅烧温度为389℃时BZF去除率预测值最高(71.29%).采用上述最佳制备条件制备的Co/RM催化臭氧氧化去除苯扎贝特的去除率为70.74%,与模型预测值十分接近,偏差为1%(<5%),说明响应面法实验设计和数学模型具有较好可靠性.通过比较RM和Co/RM两种催化剂对BZF的催化臭氧氧化去除效果,发现Co/RM催化臭氧氧化去除BZF的效果较为显著.采用BET、XRD和UV-Vis等表征手段对两种催化剂的表面结构和组成进行分析,结果表明两种催化剂的比表面积、总孔体积存在相同的变化规律(RM<Co/RM),这种变化规律与催化臭氧氧化去除BZF效果变化相一致.XRD分析结果表明,由于Co负载量小,未检测到Co氧化物的特征吸收峰.UV-Vis图谱扫描结果能够证明Co3O4的存在,Co的介入促使在RM表面形成了活性组分Co3O4,这是Co/RM表现出较高催化活性的主要原因.采用ICP-OES对RM和Co/RM催化剂催化臭氧氧化BZF溶液进行活性组分溶出情况检测,结果表明两种催化剂均没有催化活性组分溶出,说明此两种催化剂较安全,具有一定的应用前景.The removal efficiency of catalytic ozonation of bezafibrate （BZF） by red mud loaded Co catalysts （Co/RM） was used as the index value in statistical experimental designs. The most important factors influencing BZF degradation （ P 〈 0.05 ） in water were dipping mass of cobalt and calcination temperature. Under the conditions of 4. 14% of dipping mass of cobalt and 389℃ of calcination temperature, the BZF removal efficiency was 71.29% as calculated by predictive value and a maximum removal efficiency of 70. 74% was actually achieved. The experiment data was very close to the predictive value and the deviation was 1% （ 〈 5% ）. The results indicated that the response surface methodology and mathematical model was reliable for experimental design. By comparing the differences of BZF degradation in RM and Co/RM processes, it was observed that Co/RM exhibited the greater catalytic activity. Furthermore, the surface structure and composition properties of the two catalysts were evaluated by N2 adsorption, XRD and UV-Vis analysis. It was found that the specific surface area and total pore volume had the same variation trend, RM 〈 Co/RM, which was consistent with the trend of catalytic ozonation. It was also found that Co3O4 , the active component formed on the surface of RM by the addition of cobalt into red mud, enhanced the catalytic activity. Moreover, the dissolved metal concentration in the solution for catalytic ozonation of BZF degradation by RM or Co/RM was determined by 1CP-OES. The results showed that for both catalysts there was no leaching of catalytic active components into the solution, which could suggest that the two catalysts were safe and could have certain application prospect.

关 键 词：赤泥 钴 催化臭氧氧化 苯扎贝特 响应面法 

分 类 号：X703.1[环境科学与工程—环境工程]