摘要
通过浸渍-焙烧法在活性氧化铝(γ-Al_(2)O_(3))上负载稀土金属镨(Pr)制备了一种新型臭氧催化剂(Pr-Al_(2)O_(3)),研究了O_(3)/Pr-Al_(2)O_(3)系统对水中典型非甾体抗炎药(NSAIDs)阿司匹林(ASA)及非那西丁(PNT)的去除效果与机理。结果表明,两种药物的降解过程符合拟一级动力学,药物的降解速率随着pH的升高而增大、随着Pr负载量或催化剂投加量的增加呈现先增大后减小的规律。O_(3)/Pr-Al_(2)O_(3)系统降解PNT、ASA的最大拟一级动力学反应速率常数k_(obs)均发生在Pr负载浓度为5%、催化剂投加量为5 g/L、臭氧初始浓度为1.0 mg/L、pH为8.0条件下,此时k_(obs)值分别为0.1300、0.0858min^(-1)。醇抑制实验表明,催化剂提高了O_(3)降解效能是吸附和氧化协同作用的结果,且催化臭氧化产生的羟基自由基(·OH)对药物去除起主要作用。在pH为7.0条件下,·OH对ASA和PNT的降解贡献率分别为73.3%和72.1%。催化剂循环使用5次后仍保持较高的催化性能,此时系统在30 min内对ASA、PNT的去除率分别为82.4%和100%。可见,Pr-Al_(2)O_(3)催化剂是一种催化性能优异、稳定性较高的催化材料。
A novel ozone catalyst(Pr-Al_(2)O_(3))was prepared through impregnation-roasting method by loading rare earth praseodymium(Pr)on activated alumina(γ-Al_(2)O_(3)),and the performance and mechanism of the O_(3)/Pr-Al_(2)O_(3)system for the removal of typical non-steroidal anti-inflammatory drugs(NSAIDs)aspirin(ASA)and phenacetin(PNT)in water were explored.The degradation process of the two drugs conformed to the pseudo-first-order kinetic model.The degradation rate of the drugs increased with the increase of pH value,and it increased first and then decreased with the increase of Pr loading concentration or catalyst dosage.The maximum pseudo-first-order kinetic constants(k_(obs))for degradation of PNT and ASA by the O_(3)/Pr-Al_(2)O_(3)system were obtained(0.1300 min^(-1)and 0.0858 min^(-1))when the Pr loading concentration was 5%,the catalyst dosage was 5 g/L,the initial ozone concentration was 1.0 mg/L and the pH was 8.0.The alcohol inhibition experiment showed that the catalyst improved the ozone degradation efficiency due to the synergistic effect of adsorption and oxidation,and the hydroxyl radical(·OH)generated by catalytic ozonation played a major role in the drug removal.When the pH was 7.0,the contribution rate of·OH to ASA and PNT degradation was 73.3%and 72.1%,respectively.The catalyst maintained high performance after being recycled 5 times,and the removal rate of ASA and PNT were up to 82.4%and 100%respectively within 30 min.Therefore,Pr-Al_(2)O_(3)is a catalyst with excellent catalytic performance and high stability.
作者
严凯
程雪剑
崔鑫鑫
谈超群
YAN Kai;CHENG Xue-jian;CUI Xin-xin;TAN Chao-qun(Jiangsu Environmental Protection Group Co.Ltd.,Nanjing 210009,China;School of Civil Engineering,Southeast University,Nanjing 211189,China)
出处
《中国给水排水》
CAS
CSCD
北大核心
2023年第3期73-79,共7页
China Water & Wastewater
关键词
非甾体抗炎药
催化臭氧氧化
羟基自由基
拟一级动力学
non-steroidal anti-inflammatory drugs
catalytic ozonation
hydroxyl radical
pseudo-first-order kinetics
