Selective oxidation of ammonium to dinitrogen by a novel catalytic ozonation system: Regulating the N2 selectivity by sulfite.

Chemosphere Pub Date : 2025-02-01 Epub Date: 2024-12-27 DOI:10.1016/j.chemosphere.2024.143999
Yuexinxi Wang, Yong Liu, Shizong Wang, Jingwen Wang, Jianlong Wang
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Abstract

The selective oxidation of NH4+-N into dinitrogen (N2) is still a challenge. Currently, traditional advanced oxidation processes often involve in the chlorine free radicals to increase the selectivity of NH4+-N oxidation products towards N2 but is usually accompanied by the production of many toxic disinfection by-product. Herein, we reported a novel catalytic ozonation system (UV/O3/MgO/Na2SO3) for selective NH4+-N oxidation based on the reducing capability and photochemical properties of Na2SO3. In the UV/O3/MgO/Na2SO3/NH4+-N system, Na2SO3 could not only reduce the intermediate of NO2- or NO3- to N2 by inducing the generation of hydrated electrons under UV irradiation, but also reduce the gaseous intermediate of NOx to N2, thus achieving a high N2 selectivity (>85 %). Based on the analyses of each component roles, the determination of reactive oxygen species and the evolution of NH4+-N oxidation intermediates, the possible mechanisms of NH4+-N selective oxidation by UV/O3/MgO/Na2SO3 system were revealed. This system exhibits a great potential for the NH4+-N removal from water/wastewater. This work provides a new strategy for NH4+-N oxidation into N2 by advanced oxidation processes independent of the action of chlorine free radicals.

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新型催化臭氧氧化系统对氨氮的选择性氧化:亚硫酸盐对氮气选择性的调节。
NH4+-N选择性氧化成二氮(N2)仍然是一个挑战。目前,传统的高级氧化工艺通常涉及氯自由基,以增加NH4+-N氧化产物对N2的选择性,但通常伴随着许多有毒消毒副产物的产生。本文报道了一种基于Na2SO3的还原能力和光化学性质的新型臭氧氧化系统(UV/O3/MgO/Na2SO3)对NH4+-N的选择性氧化。在UV/O3/MgO/Na2SO3/NH4+- n体系中,Na2SO3不仅可以在紫外照射下通过诱导水合电子的生成将NO2-或NO3-中间体还原为N2,还可以将NOx的气态中间体还原为N2,从而实现了较高的N2选择性(> 85%)。通过对各组分作用的分析、活性氧的测定和NH4+-N氧化中间体的演化,揭示了UV/O3/MgO/Na2SO3体系选择性氧化NH4+-N的可能机理。该系统在去除水/废水中的NH4+-N方面具有很大的潜力。本研究为不依赖氯自由基的高级氧化过程将NH4+-N氧化成N2提供了一种新的策略。
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