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

IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Chemosphere Pub Date : 2025-02-01 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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来源期刊
Chemosphere
Chemosphere 环境科学-环境科学
CiteScore
15.80
自引率
8.00%
发文量
4975
审稿时长
3.4 months
期刊介绍: Chemosphere, being an international multidisciplinary journal, is dedicated to publishing original communications and review articles on chemicals in the environment. The scope covers a wide range of topics, including the identification, quantification, behavior, fate, toxicology, treatment, and remediation of chemicals in the bio-, hydro-, litho-, and atmosphere, ensuring the broad dissemination of research in this field.
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