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Cu/Mn@γ-AlO 催化臭氧氧化双酚 A:性能评价与机理洞察。

Catalytic ozonation of bisphenol A by Cu/Mn@γ-AlO: Performance evaluation and mechanism insight.

机构信息

Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, China.

School of Environment, Tsinghua University, Beijing, 100084, China.

出版信息

J Environ Manage. 2024 Jan 1;349:119403. doi: 10.1016/j.jenvman.2023.119403. Epub 2023 Oct 27.

Abstract

Herein, an alumina-based bimetallic catalyst (CuMn@γ-AlO) was synthesized for bisphenol A (BPA) degradation in the catalytic ozonation process. The catalytic ozonation system could degrade 93.9% of BPA within 30 min under the conditions of pH = 7.0, 10 mg L O concentration, and 24 g L catalyst dosage compared to ozone alone (21.0%). The enhanced BPA degradation efficiency was attributed to the abundant catalytic sites and synergistic effects of Cu and Mn. The results revealed that the synergistic interaction between Cu and Mn effectively accelerated the electron transfer process on the catalyst surface, thus promoting the generation of reactive oxygen species (ROS). Further studies indicated that the BPA degradation in CuMn@γ-AlO/O system predominantly followed the ·OH and O oxidation pathway. Based on the density functional theory (DFT) calculations and intermediates detected by LC-MS analysis, two pathways for BPA degradation in the CuMn@γ-AlO/O system were proposed. The toxicity estimation illustrated that the toxicity of BPA and its byproducts was effectively reduced in the CuMn@γ-AlO/O system. This work provides a new protocol for O activation and pollutant elimination through a novel bimetallic catalyst during water purification.

摘要

在此,我们合成了一种基于氧化铝的双金属催化剂(CuMn@γ-AlO),用于催化臭氧化过程中双酚 A(BPA)的降解。在 pH=7.0、10mg L 臭氧浓度和 24g L 催化剂剂量的条件下,催化臭氧化体系在 30 分钟内可将 BPA 降解 93.9%,而单独臭氧的降解率为 21.0%。BPA 降解效率的提高归因于丰富的催化活性位和 Cu 和 Mn 的协同作用。结果表明,Cu 和 Mn 之间的协同相互作用可有效加速催化剂表面的电子传递过程,从而促进活性氧物种(ROS)的生成。进一步的研究表明,CuMn@γ-AlO/O 体系中 BPA 的降解主要遵循·OH 和 O 氧化途径。基于密度泛函理论(DFT)计算和 LC-MS 分析检测到的中间产物,提出了 CuMn@γ-AlO/O 体系中 BPA 降解的两种途径。毒性评估表明,在 CuMn@γ-AlO/O 体系中,BPA 及其副产物的毒性得到有效降低。这项工作为通过新型双金属催化剂在水净化过程中实现 O 激活和污染物消除提供了新方案。

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