碳纳米管催化臭氧降解PFOS动力学与过程控制

臧春元; 张硕; 孙力平; 樊雪峰

doi:10.12030/j.cjee.201512059

环境工程学报

碳纳米管催化臭氧降解PFOS动力学与过程控制

, , ,

臧春元, 张硕, 孙力平, 樊雪峰. 碳纳米管催化臭氧降解PFOS动力学与过程控制[J]. 环境工程学报, 2017, 11(3): 1459-1464. doi: 10.12030/j.cjee.201512059

引用本文:

臧春元, 张硕, 孙力平, 樊雪峰. 碳纳米管催化臭氧降解PFOS动力学与过程控制[J]. 环境工程学报, 2017, 11(3): 1459-1464. doi: 10.12030/j.cjee.201512059

ZANG Chunyuan, ZHANG Shuo, SUN Liping, FAN Xuefeng. Kinetic and process control of CNT-induced catalytic ozonation of PFOS[J]. Chinese Journal of Environmental Engineering, 2017, 11(3): 1459-1464. doi: 10.12030/j.cjee.201512059

Citation:

ZANG Chunyuan, ZHANG Shuo, SUN Liping, FAN Xuefeng. Kinetic and process control of CNT-induced catalytic ozonation of PFOS[J]. Chinese Journal of Environmental Engineering, 2017, 11(3): 1459-1464. doi: 10.12030/j.cjee.201512059

碳纳米管催化臭氧降解PFOS动力学与过程控制

1.
天津城建大学环境与市政工程学院, 天津 300384
2.
天津市水质科学与技术重点实验室, 天津 300384
基金项目:
国家自然科学基金资助项目（51478292）
中图分类号: X52

Kinetic and process control of CNT-induced catalytic ozonation of PFOS

1.
School of Environmental and Municipal Engineering, Tianjin Chengjian University, Tianjin 300384, China
2.
Tianjin Key Laboratory of Aquatic Science and Technology, Tianjin 300384, China
Fund Project:

摘要: 针对全氟化合物难降解问题，通过碳纳米管（CNT）诱导臭氧高级氧化路径，研究非均相催化体系对高稳性全氟辛烷磺酸（PFOS）的降解效能与机制。结果表明：CNT介质可催化臭氧通过C-F断键对PFOS强制氧化分解，其准一级降解常数（k=0.037 min-1，5 mg·L-1 CNT）均高于碱式臭氧处理（k=0.009 min-1，pH=11）以及高负荷活性炭颗粒（k=0.013 min-1，5 g·L-1 GAC）；溶液pH是控制催化过程的重要因素，酸性或碱性环境由于PFOS吸附阻隔均不利于CNT表面与溶解O3的接触催化反应；结合羟基自由基淬灭实验，推测CNT通过表面石墨层促成·OH大量生成并在固/液界面原位降解PFOS。研究结果可为开发利用CNT介质强化臭氧水处理过程提供科学依据。
- 碳纳米管 /
- 臭氧 /
- 催化 /
- 全氟辛烷磺酸 /
- 羟基自由基
Abstract: Carbon nanotube (CNT) was utilized aiming to intensify advanced-oxidation pathway for ozonation of highly-persistent perfluorochemicals. The effectiveness on degradation of perfluorooctane sulfonate (PFOS) as model compound has been investigated in this work. Results show that CNT media can induce an intensified decomposition of PFOS through oxidative cleavage of C-F bond, of which the pseudo-first-order rate constant (k=0.037 min-1, 5 mg·L-1 CNT) is substantially higher than that of alkaline-ozonation (k=0.009 min-1, pH=11) or highly-loaded activated carbon particles (k=0.013 min-1, 5 g·L-1 GAC). Solution pH was abstracted as a controlling factor, since either acidic or basic environment was adverse to the catalytic reaction because of adsorptive hindrance of PFOS on-catalyst surface. Numerous ·OH species were speculated to generate on surface of CNT referring to ·OH scavenging experiments, and in situ interact with PFOS at solid/liquid interface. Research outcome can make referential significance for heterogeneous catalytic ozonation by virtue of CNT.
- carbon nanotube /
- ozone /
- catalysis /
- perfluorooctane sulfonate /
- hydroxyl radical

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碳纳米管催化臭氧降解PFOS动力学与过程控制

1. 天津城建大学环境与市政工程学院, 天津 300384
2. 天津市水质科学与技术重点实验室, 天津 300384

收稿日期: 2016-03-08

基金项目:

国家自然科学基金资助项目（51478292）

关键词:

摘要: 针对全氟化合物难降解问题，通过碳纳米管（CNT）诱导臭氧高级氧化路径，研究非均相催化体系对高稳性全氟辛烷磺酸（PFOS）的降解效能与机制。结果表明：CNT介质可催化臭氧通过C-F断键对PFOS强制氧化分解，其准一级降解常数（k=0.037 min-1，5 mg·L-1 CNT）均高于碱式臭氧处理（k=0.009 min-1，pH=11）以及高负荷活性炭颗粒（k=0.013 min-1，5 g·L-1 GAC）；溶液pH是控制催化过程的重要因素，酸性或碱性环境由于PFOS吸附阻隔均不利于CNT表面与溶解O3的接触催化反应；结合羟基自由基淬灭实验，推测CNT通过表面石墨层促成·OH大量生成并在固/液界面原位降解PFOS。研究结果可为开发利用CNT介质强化臭氧水处理过程提供科学依据。

English Abstract

Kinetic and process control of CNT-induced catalytic ozonation of PFOS

1. School of Environmental and Municipal Engineering, Tianjin Chengjian University, Tianjin 300384, China
2. Tianjin Key Laboratory of Aquatic Science and Technology, Tianjin 300384, China

Received Date: 2016-03-08

Fund Project:

Keywords:

Abstract: Carbon nanotube (CNT) was utilized aiming to intensify advanced-oxidation pathway for ozonation of highly-persistent perfluorochemicals. The effectiveness on degradation of perfluorooctane sulfonate (PFOS) as model compound has been investigated in this work. Results show that CNT media can induce an intensified decomposition of PFOS through oxidative cleavage of C-F bond, of which the pseudo-first-order rate constant (k=0.037 min-1, 5 mg·L-1 CNT) is substantially higher than that of alkaline-ozonation (k=0.009 min-1, pH=11) or highly-loaded activated carbon particles (k=0.013 min-1, 5 g·L-1 GAC). Solution pH was abstracted as a controlling factor, since either acidic or basic environment was adverse to the catalytic reaction because of adsorptive hindrance of PFOS on-catalyst surface. Numerous ·OH species were speculated to generate on surface of CNT referring to ·OH scavenging experiments, and in situ interact with PFOS at solid/liquid interface. Research outcome can make referential significance for heterogeneous catalytic ozonation by virtue of CNT.

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碳纳米管催化臭氧降解PFOS动力学与过程控制

Kinetic and process control of CNT-induced catalytic ozonation of PFOS

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碳纳米管催化臭氧降解PFOS动力学与过程控制

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Kinetic and process control of CNT-induced catalytic ozonation of PFOS

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