Novel method for reducing NDMA formation from daminozide during ozonation: Performances and mechanisms

IF 9.7 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Journal of Cleaner Production Pub Date : 2024-09-04 DOI:10.1016/j.jclepro.2024.143485

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Abstract

The widespread amines have been found to generate carcinogenic nitro-dimethylamine (NDMA) during ozonation, it's urgent to search effective methods to control its formation. This work investigated the performance and mechanisms of bimetallic organic framework (MIL-100(Fe-Mn)) on reducing NDMA production during ozonation of daminozide (DMNZD). The results demonstrated that NDMA concentration raised from 27.6 to 248.4 μg/L when ozone dosages enhanced from 0.5 to 4 mg/L; while just slightly increased from 0.9 to 3.7 μg/L when MIL-100 (Fe-Mn) was added, with a reduction rate up to 98.5 %. When catalyst dosages increased from 0 to 200 mg/L, NDMA reduction rates enhanced from 54.5 to 97.4%. Moreover, neutral conditions facilitated the exploitation of MIL-100(Fe-Mn) during ozonation. Water bodies containing high concentrations of CO₃²⁻, HA, and Br⁻ should be avoided to prevent high NDMA risk. MIL-100(Fe-Mn) enhanced the transformation of ozone molecular (O₃) to hydroxyl radical (·OH) other than superoxide radicals (·O₂⁻) and singlet oxygen (¹O₂). EPR and scavengers quenching experiments verified that ·OH played important roles in NDMA reduction. Except ·OH, hydrogen radicals (·H) were detected in catalyzed ozonation system for the first time. The results would provide new insights for NDMA risks control during ozonation.

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在臭氧处理过程中减少达米氮化物生成 NDMA 的新方法：性能和机理

人们发现，广泛存在的胺类物质在臭氧氧化过程中会产生致癌物质硝基二甲胺（NDMA），因此迫切需要寻找有效的方法来控制其生成。这项工作研究了双金属有机框架（MIL-100(Fe-Mn)）在减少达米诺氮化物（DMNZD）臭氧氧化过程中 NDMA 生成的性能和机理。结果表明，当臭氧用量从 0.5 mg/L 增加到 4 mg/L 时，NDMA 浓度从 27.6 μg/L 增加到 248.4 μg/L；而加入 MIL-100 (Fe-Mn)后，NDMA 浓度仅从 0.9 μg/L 轻微增加到 3.7 μg/L，降低率高达 98.5%。当催化剂用量从 0 毫克/升增加到 200 毫克/升时，NDMA 的减少率从 54.5% 提高到 97.4%。此外，中性条件有利于在臭氧处理过程中利用 MIL-100(Fe-Mn)。应避免使用含有高浓度 CO32-、HA 和 Br- 的水体，以防止出现高 NDMA 风险。除超氧自由基（-O2-）和单线态氧（1O2）外，MIL-100（Fe-Mn）还能增强臭氧分子（O3）向羟自由基（-OH）的转化。EPR 和清除剂淬灭实验证实，-OH 在 NDMA 还原过程中发挥了重要作用。除 -OH 外，催化臭氧体系中还首次检测到氢自由基（-H）。这些结果将为臭氧氧化过程中的 NDMA 风险控制提供新的启示。

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来源期刊

Journal of Cleaner Production 环境科学-工程：环境

CiteScore

20.40

自引率

9.00%

发文量

4720

审稿时长

111 days

期刊介绍： The Journal of Cleaner Production is an international, transdisciplinary journal that addresses and discusses theoretical and practical Cleaner Production, Environmental, and Sustainability issues. It aims to help societies become more sustainable by focusing on the concept of 'Cleaner Production', which aims at preventing waste production and increasing efficiencies in energy, water, resources, and human capital use. The journal serves as a platform for corporations, governments, education institutions, regions, and societies to engage in discussions and research related to Cleaner Production, environmental, and sustainability practices.