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氧化锌辅助光催化臭氧化降解全氟辛酸的机理洞察:效率与中间产物

Mechanism insight of PFOA degradation by ZnO assisted-photocatalytic ozonation: Efficiency and intermediates.

作者信息

Wu Dan, Li Xukai, Tang Yiming, Lu Ping, Chen Weirui, Xu Xiaoting, Li Laisheng

机构信息

School of Chemistry & Environment, South China Normal University, Guangzhou 510006, China.

School of Chemistry & Environment, South China Normal University, Guangzhou 510006, China; Guangdong Provincial Engineering Technology Research Center for Drinking Water Safety, Guangzhou 510006, China; Guangdong Provincial Key Lab of Functional Materials for Environmental Protection, Guangzhou 510006, China.

出版信息

Chemosphere. 2017 Aug;180:247-252. doi: 10.1016/j.chemosphere.2017.03.127. Epub 2017 Apr 3.

Abstract

Zinc oxide (ZnO) nanorods were prepared by a directly pyrolysis method and employed as catalyst for perfluorooctanoic acid (PFOA) degradation. Comparative experiments were conducted to discuss the catalytic activity and flexibility of ZnO. After ZnO addition, the best PFOA degradation efficiency (70.5%) was achieved by ZnO/UV/O system, only 9.5% by sole ozonation and 18.2% by UV light irradiation. PFOA degradation was sensitive with pH value and temperature. The better PFOA removal efficiency was achieved at acidic condition. A novel relationship was found among PFOA degradation efficiency with hydroxyl radicals and photo-generated holes. Hydroxyl radicals generated on the surfaces of ZnO nanorods played dominant roles in PFOA degradation. PFOA degradation was found to follow the photo-Kolbe reaction mechanism. C-C shorter-chain perfluorocarboxylic acids and fluoride ion were detected as main intermediates during PFOA degradation process. Based on the results, a proposal degradation pathway was raised.

摘要

采用直接热解方法制备了氧化锌(ZnO)纳米棒,并将其用作全氟辛酸(PFOA)降解的催化剂。进行了对比实验以探讨ZnO的催化活性和灵活性。添加ZnO后,ZnO/UV/O体系实现了最佳的PFOA降解效率(70.5%),单独臭氧氧化的降解效率为9.5%,紫外光照射的降解效率为18.2%。PFOA降解对pH值和温度敏感。在酸性条件下实现了更好的PFOA去除效率。发现了PFOA降解效率与羟基自由基和光生空穴之间的新关系。ZnO纳米棒表面产生的羟基自由基在PFOA降解中起主导作用。发现PFOA降解遵循光科尔贝反应机理。在PFOA降解过程中,检测到C-C短链全氟羧酸和氟离子为主要中间体。基于这些结果,提出了一条可能的降解途径。

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