School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou 510006, P. R. China.
Department of Chemistry, College of Sciences, Shanghai University, Shanghai 200444, P. R. China.
Environ Sci Technol. 2023 May 2;57(17):7041-7050. doi: 10.1021/acs.est.2c08867. Epub 2023 Apr 20.
Ozone catalytic oxidation (OZCO) has gained great interest in environmental remediation while it still faces a big challenge during the deep degradation of refractory volatile organic compounds (VOCs) at room temperature. Hydroxylation of the catalytic surface provides a new strategy for regulating the catalytic activity to boost VOC degradation. Herein, OZCO of toluene at room temperature over hydroxyl-mediated MnO/AlO catalysts was originally demonstrated. Specifically, a novel hydroxyl-mediated MnO/AlO catalyst was developed via the in situ AlOOH reconstruction method and used for toluene OZCO. The toluene degradation performance of MnO/AlO was significantly superior to those of most of the state-of-the-art catalysts, and 100% toluene was removed with an excellent mineralization rate (82.3%) and catalytic stability during OZCO. ESR and in situ DRIFTs results demonstrated that surface hydroxyl groups (HGs) greatly improved the reactive oxygen species generation, thus dramatically accelerating the benzene ring breakage and deep mineralization. Furthermore, HGs provided anchoring sites for uniformly dispersing MnO and greatly enhanced toluene adsorption and ozone activation. This work paves a way for deep decomposition of aromatic VOCs at room temperature.
臭氧催化氧化(OZCO)在环境修复方面引起了极大的关注,但在室温下深度降解难挥发性挥发性有机化合物(VOCs)时仍面临巨大挑战。催化表面的羟化作用为调节催化活性以促进 VOC 降解提供了新策略。本文首次在室温下通过羟基介导的 MnO/AlO 催化剂展示了甲苯的 OZCO。具体而言,通过原位 AlOOH 重构方法开发了一种新型的羟基介导的 MnO/AlO 催化剂,并将其用于甲苯的 OZCO。与大多数最先进的催化剂相比,MnO/AlO 的甲苯降解性能明显优越,在 OZCO 过程中,甲苯的去除率达到 100%,矿化率(82.3%)和催化稳定性均优异。ESR 和原位 DRIFTs 结果表明,表面羟基(HGs)极大地提高了活性氧物种的生成,从而显著加速了苯环断裂和深度矿化。此外,HGs 为均匀分散的 MnO 提供了锚定位点,极大地增强了甲苯的吸附和臭氧的活化。这项工作为室温下芳香族 VOC 的深度分解铺平了道路。