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无曝气原位类芬顿反应:异相氧空位对氧的特异性吸附与活化

Aeration-Free In Situ Fenton-like Reaction: Specific Adsorption and Activation of Oxygen on Heterophase Oxygen Vacancies.

机构信息

State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, Heilongjiang Province 150090, China.

出版信息

Environ Sci Technol. 2024 Jan 30;58(4):1921-1933. doi: 10.1021/acs.est.3c08579. Epub 2024 Jan 17.

Abstract

Aeration accounts for 35-51% of the overall energy consumption in wastewater treatment processes and results in an annual energy consumption of 5-7.5 billion kWh. Herein, a solar-powered continuous-flow device was designed for aeration-free in situ Fenton-like reactions to treat wastewater. This system is based on the combination of TiO/WO featuring heterophase oxygen vacancy interactions with floating reduced graphene/polyurethane foam, which produces hydrogen peroxide in situ at the rates of up to 4.2 ppm h with degradation rates of more than 90% for various antibiotics. The heterophase oxygen vacancies play an important role in the stretching of the O-O bond by regulating the d-band center of TiO/WO, promoting the hydrogenation of *·O or *OOH by H enrichment, and accelerating the production of reactive oxygen species by spontaneous adsorption of hydrogen peroxide. Furthermore, the degradation mechanisms of antibiotics and the treatment of actual wastewater were thoroughly investigated. In short, the study provides a meaningful reference for potentially undertaking the "aeration-free" in situ Fenton reaction, which can help reduce or even completely eradicate the aeration costs and energy requirements during the treatment of wastewater.

摘要

曝气占废水处理过程总能耗的 35-51%,导致每年的能耗为 5-75 亿千瓦时。在此,设计了一种太阳能驱动的连续流动装置,用于无曝气的原位芬顿样反应来处理废水。该系统基于 TiO/WO 与漂浮还原氧化石墨烯/聚氨酯泡沫的异质相氧空位相互作用相结合,可原位产生高达 4.2 ppm h 的过氧化氢,各种抗生素的降解率超过 90%。异质相氧空位通过调节 TiO/WO 的 d 带中心来拉伸 O-O 键,促进 H 富集时的 *·O 或 *OOH 加氢,并通过过氧化氢的自发吸附加速活性氧物质的产生,在这一过程中发挥着重要作用。此外,还深入研究了抗生素的降解机制和实际废水的处理。总之,该研究为潜在的“无曝气”原位芬顿反应提供了有意义的参考,可以帮助减少甚至完全消除废水处理过程中的曝气成本和能源需求。

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