水动力空化与过硫酸盐 Fenton 类过程协同增强双酚 A 降解:空化气泡在调节反应途径中作用的新见解

IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2024-10-19 DOI:10.1016/j.watres.2024.122666
Hongkun Han, Mengfan Chen, Congting Sun, Yuying Han, Lanlan Xu, Yingming Zhao
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引用次数: 0

摘要

流体动力空化(HC)与 Fenton 类氧化技术相结合可显著提高污染物的去除能力,但空化与催化剂对活性氧(ROS)生成的协同效应仍是一个谜。在本研究中,我们建立了一个基于碳氢化合物和 Ce-MnFe2O4 活化过一硫酸盐(PMS)的组合系统来去除双酚 A,并关注了空化气泡的作用。研究结果表明,在 Ce-MnFe2O4 活化的 PMS 中加入碳氢化合物,可将双酚 A 的降解途径从以 1O2 为主的非自由基途径转变为以 -O2- 为主的自由基途径。对照实验和理论计算都表明,不同大小的空化气泡在 ROS 生成中起着主导作用。空化气泡坍塌产生的微射流可在 Ce-MnFe2O4 表面产生大量氧空位缺陷,从而改变 PMS 的活化势垒,从热力学角度促进 -O2- 的生成。稳定存在的空化气泡大小为 100∼400 nm,可形成相当大的气液界面。分子动力学模拟结果表明,纳米气泡可以浓缩双酚 A,增加双酚 A 与 Ce-MnFe2O4 接触的几率,从而有效地解决了 -O2- 自由基寿命短和传质距离有限的问题,强化了反应。此外,PMS/Ce-MnFe2O4/HC 系统不仅达到了令人满意的 COD(95%)和 TOC(65%)去除率,而且以 0.065 kWh-m-3 的低能耗成本和低氧化剂成本处理了双酚 A 污染水,凸显了 HC 技术在污染水领域的应用潜力。
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Synergistic Enhancement in Hydrodynamic Cavitation combined with Peroxymonosulfate Fenton-like Process for BPA Degradation: New Insights into the Role of Cavitation Bubbles in Regulation Reaction Pathway
The combination of hydrodynamic cavitation (HC) and Fenton-like oxidation technology can dramatically enhance the pollutant removal capacity, however, the synergistic effect of cavitation and catalyst on reactive oxygen species (ROS) generation remained enigmatic. In this study, we established a combined system based on HC and Ce-MnFe2O4 activated peroxymonosulfate (PMS) for BPA removal, and attentions were paid on the role of cavitation bubbles. Study results show that the combination of HC in Ce-MnFe2O4 activated PMS could mediate the degradation of BPA from the non-radical pathway dominated by 1O2 to •O2 dominated radical pathway. Both controlled experiments and theoretical calculations revealed that the cavitation bubbles with different sizes play the dominant role in ROS generation. The microjets produced by the collapse of cavitation bubbles could create a large number of oxygen vacancy defects on Ce-MnFe2O4 surface, which modify the activation barrier of PMS and facilitate the generation of •O2 thermodynamically. The stable existing cavitation bubbles with the size of 100∼400 nm could create considerable gas-liquid interface. The molecular dynamics simulations show that the nano bubbles can concentrate the BPA and increase the probability of contacts between BPA and Ce-MnFe2O4, hence effectively solve the issues of short lifetime of •O2 radicals and limited mass transfer distance to strengthen the reaction. In addition, the PMS/Ce-MnFe2O4/HC system not only achieves the satisfied COD (95%) and TOC (65%) removal efficiency but also enabled the BPA-contaminated water with a low energy cost of 0.065 kWh·m−3 and oxidant cost, highlighting the application potential of the HC technology for contaminated water.
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来源期刊
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
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