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Catalytic oxidation of sulfachloropyridazine by MnO2: Effects of crystalline phase and peroxide oxidants
Chemosphere ( IF 8.1 ) Pub Date : 2020-12-11 , DOI: 10.1016/j.chemosphere.2020.129287
Jianchao Ma , Siyu Zhang , Xiaoguang Duan , Yuxin Wang , Danlei Wu , Jin Pang , Xin Wang , Shaobin Wang

Catalytic activation of different oxidants including peroxymonosulfate (PMS), peroxydisulfate (PDS), hydrogen peroxide (H2O2) and ozone (O3) by MnO2 for degradation of sulfachloropyridazine (SCP) was investigated and the effects of different crystalline phases of MnO2 including nanowire α-MnO2, nanorod β-MnO2, nanofiber γ-MnO2, and nanosphere δ-MnO2 on catalytic ozonation of SCP were also studied. The SCP degradation and total organic carbon removal indicated that the oxidation efficiency of the peroxide oxidants followed an order of O3/MnO2 > PMS/MnO2 > PDS/MnO2 > H2O2/MnO2. In catalytic ozonation, SCP degradation rate constants of different MnO2 phases followed an order of δ-MnO2 > α-MnO2 > γ-MnO2> β-MnO2. Electron paramagnetic resonance (EPR) suggested that hydroxyl radicals (·OH) and singlet oxygen (1O2) might be more significant for SCP degradation than sulfate (SO4·−) and superoxide (·O2) radicals. Radical competition experiments demonstrated that 1O2 and ·OH contributed to 63.16% and 28.07%, respectively, for the catalytic ozonation of SCP. It was also found that more oxygen vacancies, specific surface area and exposure of MnO6 edges could facilitate the activation of O3 for 1O2 and ·OH productions and SCP degradation. The degradation pathways of SCP could mainly follow the cleavage of S–C or S–N bond and dechlorination, accompanied by hydroxylation and oxidation.



中文翻译:

MnO 2催化氧化磺胺氯哒嗪:晶相和过氧化物氧化剂的影响

研究了MnO 2对包括过氧一硫酸盐(PMS),过氧二硫酸盐(PDS),过氧化氢(H 2 O 2)和臭氧(O 3)的不同氧化剂的催化活化对磺胺氯哒嗪(SCP)的降解作用,并考察了不同结晶相的影响。的MnO 2包括纳米线α-MnO的2,纳米棒β-MnO的2,纳米纤维γ-MnO的2,和纳米球δ-的MnO 2上SCP的催化臭氧化也进行了研究。SCP降解和总有机碳去除表明,过氧化物氧化剂的氧化效率遵循O 3 / MnO 2  > PMS / MnO的顺序。2  > PDS / MnO 2  > H 2 O 2 / MnO 2。在催化臭氧化,不同的MnO SCP降解速率常数2相,随后的顺序δ-的MnO 2  >α-MnO的2  >γ-MnO的2 >β-MnO的2。电子顺磁共振(EPR)表明,羟基自由基(·OH)和单线态氧(1 O 2)对于SCP降解可能比硫酸盐(SO 4 ·−)和超氧自由基(·O 2 )更为重要。激进竞争实验表明1 O 2·OH对SCP的催化臭氧化作用分别占63.16%和28.07%。人们还发现,更氧空位,比表面积和MnO的曝光6边缘可以方便的O活化31 Ò 2和·OH制作和SCP降解。SCP的降解途径可能主要是通过S–C或S–N键的裂解和脱氯,再伴随有羟基化和氧化。

更新日期:2020-12-18
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