使用羟基介导的 MnOx/Al2O3 催化剂在室温下促进甲苯的臭氧催化氧化,Environmental Science & Technology

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使用羟基介导的 MnOx/Al2O3 催化剂在室温下促进甲苯的臭氧催化氧化
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2023-04-20 , DOI: 10.1021/acs.est.2c08867
Boge Zhang ₁ , Yongjie Shen ₂ , Biyuan Liu ₁ , Jian Ji ₃ , Wenjing Dai ₁ , Pingli Huang ₁ , Dengsong Zhang ₂ , Guangqin Li ₁ , Ruijie Xie ₁ , Haibao Huang ₁

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臭氧催化氧化（OZCO）在环境修复中引起了极大的兴趣，但在室温下难降解挥发性有机化合物（VOCs）的深度降解过程中仍然面临着巨大的挑战。催化表面的羟基化为调节催化活性以促进 VOC 降解提供了一种新策略。在此，最初展示了甲苯在室温下通过羟基介导的 MnO _x /Al ₂ O _{3催化剂的 OZCO。}具体而言，通过原位 AlOOH 重构方法开发了一种新型羟基介导的 MnO _x /Al ₂ O _{3催化剂，并将其用于甲苯 OZCO。}_{MnO x} /Al的甲苯降解性能₂ O ₃明显优于大多数最先进的催化剂，在 OZCO 过程中，100% 的甲苯被去除，并具有出色的矿化率 (82.3%) 和催化稳定性。ESR 和原位 DRIFT 结果表明，表面羟基 (HGs) 极大地提高了活性氧的产生，从而显着加速了苯环断裂和深层矿化。_{此外，HGs 为均匀分散MnOx}提供了锚定位点，并大大增强了甲苯吸附和臭氧活化。这项工作为在室温下深度分解芳香族 VOC 铺平了道路。

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Boosting Ozone Catalytic Oxidation of Toluene at Room Temperature by Using Hydroxyl-Mediated MnOx/Al2O3 Catalysts

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_x/Al₂O₃ catalysts was originally demonstrated. Specifically, a novel hydroxyl-mediated MnO_x/Al₂O₃ catalyst was developed via the in situ AlOOH reconstruction method and used for toluene OZCO. The toluene degradation performance of MnO_x/Al₂O₃ 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_x and greatly enhanced toluene adsorption and ozone activation. This work paves a way for deep decomposition of aromatic VOCs at room temperature.

更新日期：2023-04-20

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