Self-Accelerating Interfacial Catalytic Elimination of Gaseous Sulfur-Containing Volatile Organic Compounds as Microbubbles in a Facet-Engineered Three-Dimensional BiOCl Sponge Fenton-Like Process
Self-Accelerating Interfacial Catalytic Elimination of Gaseous Sulfur-Containing Volatile Organic Compounds as Microbubbles in a Facet-Engineered Three-Dimensional BiOCl Sponge Fenton-Like Process
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在面工程三维 BiOCl 海绵类芬顿过程中以微泡形式自加速界面催化消除气态含硫挥发性有机化合物
DOI：
10.1021/acs.est.2c01798
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Dong Shu
中科院分区：
文献类型：
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作者：
Wei Qu;Zhuoyun Tang;Wei Liu;Yuhong Liao;Yajing Huang;Dehua Xia;Qiyu Lian;Shuanghong Tian;Chun He;Dong Shu
利用微泡辅助的类Fenton法去除气态含硫挥发性有机化合物（S-VOCs）是一种创新的方法。在此，我们建立了一个微泡辅助Fenton类过程，以消除恶臭微泡CH 3SH作为代表性的气态S-VOCs，其中BiOCl纳米片负载在三维海绵暴露于（001）或（010）面，并诱导Fenton类界面反应。有趣的是，微泡辅助的类Fenton过程显著去除了99.9%的CH 3SH，高于大泡辅助的类Fenton过程（39.0%）。通过原位ATR-FTIR、PTR-TOF-MS、EPR和DFT计算研究，深入探讨了自加速界面催化机理。微泡辅助类Fenton过程的优异去除性能在于其提高了气相CH 3SH在气/液相中的溶解/传质能力，以及微泡上升速度较低使CH 3SH与3D-BiOCl海绵紧密接触（0.13 mm s-1）和负电荷（-45.53 mV）的CH 3SH-微泡，以及通过3D-BiOCl海绵上的有效电子极化位点激活CH_3SH-微泡中富集的溶解氧而有效产生1 O_2。此外，CH 3SH-微泡通过3D-BiOCl海绵的富电子氧空位中心向H2 O2传递电子，产生更多的·OH，从而实现优异的消除性能。总之，本研究证明了增强的自加速界面催化消除S-VOC微泡，并提供了潜在的机制。
The elimination of gaseous sulfur-containing volatile organic compounds (S-VOCs) by a microbubble-assisted Fenton-like process is an innovative strategy. Herein, we established a microbubble-assisted Fenton-like process to eliminate malodorous microbubble CH3SH as representative gaseous S-VOCs, in which BiOCl nanosheets loaded on a three-dimensional sponge were exposed to (001) or (010) facets and induced Fenton-like interface reactions. Intriguingly, the microbubble-assisted Fenton-like process significantly removed 99.9% of CH3SH, higher than that of the macrobubble-assisted Fenton-like process (39.0%). The self-accelerating interfacial catalytic mechanism was in-depth identified by in situ ATR-FTIR, PTR-TOF-MS, EPR, and DFT computational study. The extraordinary elimination performance of microbubble-assisted Fenton-like process lies in the enhancing dissolution/mass transfer of gaseous CH3SH in the gas/liquid phase and the tight contact between CH3SH-microbubbles and 3D-BiOCl sponge due to the low rising velocity (0.13 mm s-1) and negative charge (-45.53 mV) of CH3SH-microbubbles, as well as the effective generation of 1O2 by activating the enriched dissolved oxygen in CH3SH-microbubble via effective electron-polarized sites on 3D-BiOCl sponge. Furthermore, CH3SH-microbubbles transferred electrons to H2O2 through electron-rich oxygen vacancy centers of the 3D-BiOCl sponge to generate more •OH, thus achieving excellent elimination performance. Overall, this study demonstrates the enhanced self-accelerating interfacial catalytic elimination by S-VOC microbubble and provides the underlying mechanisms.