Simultaneous Oxidation of Bromide and Dissolution of Manganese Oxide Induced by Freezing

IF 10.8 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

环境科学与技术 Pub Date : 2024-09-24 DOI:10.1021/acs.est.4c07493

Yaohua Wu, Huazhe Wang, Juanshan Du, Yi Hu, Qinglian Wu, Wanqian Guo, Wonyong Choi

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引用次数: 0

Abstract

This study demonstrates that the oxidation of bromide by birnessite (δ-MnO₂) results in the concurrent production of soluble manganese (Mn(II)) and reactive bromine (RBr) species in frozen solutions, a process not observed in aqueous solutions. This enhanced oxidation in ice is attributed to the concentration of protons, birnessite, or bromide in the ice grain boundary region. Furthermore, different types of commercial manganese oxides can also oxidize bromide to RBr and release Mn(II) in ice. The presence of fulvic acid (FA) further increases the simultaneous production of RBr and Mn(II) in ice, accompanying the formation of organobromine compounds (OBCs). In frozen δ-MnO₂/Br^–/FA system, a significant increase in OBCs, mainly highly unsaturated and phenolic compounds, was detected using Fourier transform ion cyclotron resonance mass spectrometry. A marked contrast was observed in the number of OBCs formed in frozen solutions (853 and 415 OBCs at initial pH 3.0 and 5.8, respectively) compared to their aqueous counterparts (11 and 23 OBCs). These findings introduce a new pathway for the formation of RBr, Mn(II), and OBCs in ice, highlighting the need for further research on the environmental fate of bromide and manganese.

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冷冻引起的溴化物同时氧化和氧化锰溶解

这项研究证明，在冰冻溶液中，桦锰矿（δ-MnO2）氧化溴化物会同时产生可溶性锰（Mn(II)）和活性溴（RBr）物种，而这是在水溶液中观察不到的过程。冰中氧化作用的增强归因于冰粒边界区域的质子、桦锰酸盐或溴化物的浓度。此外，不同类型的商用锰氧化物也能将溴氧化成 RBr，并在冰中释放出 Mn（II）。富勒酸（FA）的存在进一步增加了冰中 RBr 和 Mn（II）的同时生成，并伴随着有机溴化合物（OBCs）的形成。在冷冻的δ-MnO2/Br-/FA 系统中，利用傅立叶变换离子回旋共振质谱法检测到 OBCs 显著增加，主要是高度不饱和和酚类化合物。在冷冻溶液中形成的 OBC 数量（初始 pH 值为 3.0 和 5.8 时分别为 853 和 415 OBC）与水溶液中形成的 OBC 数量（11 和 23 OBC）形成了明显的对比。这些发现为冰中溴化钾、锰（II）和 OBC 的形成提供了新的途径，强调了进一步研究溴和锰的环境归宿的必要性。

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来源期刊

环境科学与技术环境科学-工程：环境

CiteScore

17.50

自引率

9.60%

发文量

12359

审稿时长

2.8 months

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. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.