Han Hongkun, Chen Mengfan, Sun Congting, Han Yuying, Xu Lanlan, Zhao Yingming
School of Environment, Liaoning University, Liaoning Province, Shenyang 110036, PR China.
School of Environment, Liaoning University, Liaoning Province, Shenyang 110036, PR China.
Water Res. 2025 Jan 1;268(Pt A):122666. doi: 10.1016/j.watres.2024.122666. Epub 2024 Oct 19.
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 catalysts on reactive oxygen species (ROS) generation remained enigmatic. In this study, we established a combined system based on HC and Ce-MnFeO activated peroxymonosulfate (PMS) for BPA removal, and attentions were paid on the role of cavitation bubbles. The results show that the combination of HC in Ce-MnFeO activated PMS could mediate the degradation of BPA from the non-radical pathway dominated by O to •O 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-MnFeO surface, which modify the activation barrier of PMS and facilitate the generation of •O 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-MnFeO, hence effectively solve the issues of short lifetime of •O radicals and limited mass transfer distance to strengthen the reaction. In addition, the PMS/Ce-MnFeO/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 and oxidant cost, highlighting the application potential of the HC technology for contaminated water.
水力空化（HC）与类芬顿氧化技术相结合可显著提高污染物去除能力，然而，空化与催化剂对活性氧（ROS）生成的协同作用仍不清楚。在本研究中，我们建立了基于HC和Ce-MnFeO活化过一硫酸盐（PMS）的联合体系用于去除双酚A（BPA），并关注空化气泡的作用。结果表明，HC与Ce-MnFeO活化PMS相结合可介导BPA的降解从以O为主的非自由基途径转变为以•O为主的自由基途径。对照实验和理论计算均表明，不同尺寸的空化气泡在ROS生成中起主导作用。空化气泡崩溃产生的微射流可在Ce-MnFeO表面产生大量氧空位缺陷，改变PMS的活化能垒并在热力学上促进•O的生成。尺寸为100∼400 nm的稳定存在的空化气泡可形成可观的气液界面。分子动力学模拟表明，纳米气泡可浓缩BPA并增加BPA与Ce-MnFeO之间的接触概率，从而有效解决•O自由基寿命短和传质距离有限的问题以强化反应。此外，PMS/Ce-MnFeO/HC体系不仅实现了令人满意的化学需氧量（COD）去除率（95%）和总有机碳（TOC）去除率（65%），还使受BPA污染的水的能源成本低至0.065 kWh·m且氧化剂成本低，突出了HC技术在处理受污染水体方面的应用潜力。
