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真空紫外/亚硫酸盐体系高效还原溴酸盐。

Highly efficient reduction of bromate by vacuum UV/sulfite system.

机构信息

School of Environment, Harbin Institute of Technology, Harbin, 150090, PR China.

College of Environment and Ecology, Chongqing University, Chongqing, 400045, PR China.

出版信息

Chemosphere. 2024 Feb;349:140875. doi: 10.1016/j.chemosphere.2023.140875. Epub 2023 Dec 7.

Abstract

Bromate (BrO3-), a worldwide regulated by-product after ozone disinfection, is often detected in bromide-containing water, and has a strict limit of 10 μg L in potable water. BrO3- degradation by advanced reduction processes (ARPs) has gained much attention because of efficient removal and easy integration with ultraviolet disinfection (UV at 254 nm). In the vacuum UV (VUV, 185/254 nm)/sulfite system, the elimination kinetics of BrO increased by 9-fold and 15-fold comparing with VUV alone and UV/sulfite system. This study further demonstrated the hydrated electron (eaq-) works as the dominant species in BrO3- degradation in alkaline solution, while in the acidic solution the H• became a secondary reactive species besides e. Hence, the influences of pH, sulfite concentration, dissolved gas and water matrix on effectiveness of degradation kinetics of BrO3- was explored in details. With increasing pH, the proportion of SO species increased and even became the major ones, which also correlated well with the k (min) of BrO degradation. The stability of e also climbs with increasing pH, while that of H• drops significantly. Higher sulfite dosage favored a more rapid degradation of BrO. The presence of dissolved oxygen inhibited BrO3- removal due to the scavenging effect of O toward e and transformed VUV/sulfite-based ARP to an advanced oxidation process (AOP), which was ineffective for BrO3- removal. BrO3- removal was inhibited to varying degrees after anions (e.g., bicarbonate (HCO), chloride (Cl), nitrate (NO)) and humic acid (HA) being added.

摘要

溴酸盐(BrO3-)是臭氧消毒后的一种全球监管副产物,常存在于含溴水中,饮用水中的限量为 10μg/L。由于高效去除和易于与紫外线消毒(254nm 紫外光)集成,高级还原工艺(ARPs)对 BrO3-的降解受到了广泛关注。在真空紫外(VUV,185/254nm)/亚硫酸盐体系中,与单独 VUV 和 UV/亚硫酸盐体系相比,BrO 的消除动力学提高了 9 倍和 15 倍。本研究进一步证明了在碱性溶液中,电子空穴(eaq-)是 BrO3-降解的主要物种,而在酸性溶液中,H•除了 e 之外也是一种次要活性物质。因此,详细探讨了 pH 值、亚硫酸盐浓度、溶解气体和水基质对 BrO3-降解动力学效果的影响。随着 pH 值的增加,SO 物种的比例增加,甚至成为主要物种,这也与 BrO 降解的 k(min)很好地相关。电子空穴的稳定性随 pH 值的增加而增加,而 H•的稳定性则显著降低。较高的亚硫酸盐用量有利于 BrO 的快速降解。溶解氧的存在由于 O 对 e 的清除作用而抑制了 BrO3-的去除,将 VUV/亚硫酸盐基 ARP 转变为一种无效的 BrO3-去除的高级氧化过程(AOP)。阴离子(如碳酸氢根(HCO)、氯离子(Cl)、硝酸根(NO))和腐殖酸(HA)的存在会不同程度地抑制 BrO3-的去除。

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