酸活化赤泥催化臭氧氧化降解水中硝基苯的效能研究

Catalytic Ozonation of Nitrobenzene in Water by Acidification-activated Red Mud

以铝工业废物赤泥为原料,采用酸化的方法活化赤泥,提高其在多相催化臭氧氧化除污染体系中的催化活性,并对其催化臭氧除污染效能及机制进行探讨.研究发现,和赤泥原矿相比,酸化赤泥表现出十分显著的催化能力;酸化赤泥(RM6.0)催化臭氧氧化硝基苯的去除率随臭氧浓度的增加而增加;当臭氧浓度由0.4 mg.L-1增加至1.7 mg.L-1时,硝基苯的去除率由45%提高到92%.溶液pH对RM6.0催化体系利用臭氧能力的影响与其催化臭氧氧化降解NB的影响表现出一致的结果.初始pH变化所带来的RM6.0催化活性的变化,主要是由于体系中氢氧根浓度的变化,导致臭氧分解形成羟基自由基所致;过高pH值导致的羟基自由基的猝灭显促使RM6.0催化臭氧氧化NB活性的降低.通过RM6.0对臭氧的利用能力及羟基自由基抑制实验结果发现,RM6.0催化臭氧降解NB的主要作用机制是催化剂表面吸附臭氧,实现臭氧在催化剂表面的富集,进而实现对NB有机污染物的氧化降解.在这个过程中羟基自由基是存在的,主要是在臭氧与硝基苯在界面氧化过程中分解而成,并进一步氧化NB.

Red mud as one kind of aluminum industrial wastes was used as raw material for catalyst preparation.It was activated by acidification in order to enhance its catalytic activity in the system of catalytic ozonation.Furthermore,removal performance and reaction mechanism in degradation of organic pollutants were discussed.Results showed that acid modified red mud had more significant catalytic activity than the raw red mud.The removal efficiency of nitrobenzene by catalytic ozonation with acidified red mud（RM6.0） increased with the increasing ozone concentration.When the ozone concentration was increased from 0.4 mg·L^-1 to 1.7 mg·L^-1,the removal efficiency of nitrobenzene increased from 45% to 92%.There was a consistent effect of water pH on the removal efficiency and the ozone concentration variation.The variation of the removal efficiency depended on the initial water pH.This was because the concentration of OH-led to ozone decomposition to generate hydroxyl radicals.The higher water pH value led to the quenching of hydroxyl radicals,resulting in the reduction of catalytic activity of RM6.0.The experimental results of aqueous ozone concentration variation in the presence of RM6.0 and inhibition by hydroxyl radicals indicated that the main reaction mechanism was catalytic ozonation of NB.Firstly,aqueous ozone was absorbed onto the surface of RM6.0,and then the concentrated ozone oxidized NB in water which was with a combination of direct and indirect oxidation.In catalytic reaction,hydroxyl radicals were present,which were generated during the oxidation of NB on the surface of RM6.0.