Yinhao Dai, , , Fuqiang Liu, , , Zhenhua Dai, , , Wei Miao, , , Hongyu Dong*, , , Irene M. C. Lo, , and , Xiaohong Guan*,
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Increasing the salinity from 15 to 200 g L<sup>–1</sup> significantly inhibited OA removal in the CuO/O<sub>3</sub> system, while no inhibitory effect was observed in the other three systems. Mechanistic studies revealed that Cl<sup>–</sup> inhibited OA removal in the CuO/O<sub>3</sub> system by quenching the aqueous-phase hydroxyl radicals (HO<sub>aq</sub><sup>•</sup>). Although HO<sub>aq</sub><sup>•</sup> was also the dominant oxidant in both Mn<sub>2</sub>O<sub>3</sub>/O<sub>3</sub> and Fe<sub>3</sub>O<sub>4</sub>/O<sub>3</sub> systems, their negatively charged surfaces electrostatically repelled Cl<sup>–</sup>, preventing the depletion of HO<sub>aq</sub><sup>•</sup> by Cl<sup>–</sup> and thus maintaining the catalytic activity. Differently, surface-adsorbed hydroxyl radicals were generated in the CuO/MnO<sub>2</sub>/O<sub>3</sub> system, enabling the salt-resistance performance of this system. 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引用次数: 0
摘要
由于对其耐盐机制的了解有限,选择有效的臭氧催化剂用于高盐废水处理仍然是一个重大挑战。本文筛选了24种商用臭氧催化剂(标记为#1-#24)的耐盐催化性能,其中4种催化剂(#1,#15,#22和#23)在15 g L-1 NaCl存在下表现出优异的草酸(OA)的催化臭氧化活性。四种催化剂的活性组分分别为CuO(#1)、CuO/MnO2(#15)、Mn2O3(#22)和Fe3O4(#23)。盐度从15 g L-1增加到200 g L-1显著抑制CuO/O3体系对OA的去除,而对其他3个体系无抑制作用。机理研究表明,Cl-通过猝灭水相羟基自由基(HOaq•)抑制CuO/O3体系中OA的去除。虽然在Mn2O3/O3和Fe3O4/O3体系中,HOaq•也是主要的氧化剂,但它们带负电荷的表面静电排斥Cl-,防止了Cl-对HOaq•的消耗,从而保持了催化活性。不同的是,在CuO/MnO2/O3体系中产生了表面吸附的羟基自由基,使该体系具有耐盐性能。本研究为高盐废水催化臭氧化的有效催化剂的选择和设计铺平了道路。
Mechanistic Insights into Salt Resistance of Commercial Ozone Catalysts for Hypersaline Wastewater Decontamination
The selection of effective ozone catalysts for hypersaline wastewater treatment remains a significant challenge due to the limited understanding of their salt-resistance mechanisms. Herein, 24 commercial ozone catalysts (denoted as #1–#24) were screened for salt-resistant catalytic performance, among which four catalysts (#1, #15, #22, and #23) demonstrated exceptional catalytic ozonation activity for oxalate (OA) removal in the presence of 15 g L–1 NaCl. The active components of these four catalysts were identified as CuO (#1), CuO/MnO2 (#15), Mn2O3 (#22), and Fe3O4 (#23), respectively. Increasing the salinity from 15 to 200 g L–1 significantly inhibited OA removal in the CuO/O3 system, while no inhibitory effect was observed in the other three systems. Mechanistic studies revealed that Cl– inhibited OA removal in the CuO/O3 system by quenching the aqueous-phase hydroxyl radicals (HOaq•). Although HOaq• was also the dominant oxidant in both Mn2O3/O3 and Fe3O4/O3 systems, their negatively charged surfaces electrostatically repelled Cl–, preventing the depletion of HOaq• by Cl– and thus maintaining the catalytic activity. Differently, surface-adsorbed hydroxyl radicals were generated in the CuO/MnO2/O3 system, enabling the salt-resistance performance of this system. This work paves the way for both selecting and designing effective catalysts for catalytic ozonation of hypersaline wastewater.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
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