Titanium carbide MXene/anatase titanium dioxide-supported gold catalysts for the low-temperature oxidation of benzene in indoor air

초록

In the present study, the oxidative removal of benzene (model carcinogenic aromatic volatile organic compound (VOC)) from indoor air is investigated using titanium carbide (Ti3C2) MXene/anatase titanium dioxide (TiO2)-supported gold (Au) catalysts under dark and low-temperature (DLT: 30–90 °C) conditions. The reduction pre-treatment (catalyst labelled with the ‘R’ suffix) has been used to form metallic Au (Au0) nanoparticles and anatase TiO2 in the MXene structure. The relative ordering in the Au catalysts, if assessed in terms of room-temperature (RT) benzene (5 ppm) conversion (XB (%)) at 10,191 h−1 gas hourly space velocity, is found as: 0.5 %-Au/Ti3C2-R (85 ± 5.5 %) > 0.2 %-Au/Ti3C2-R (71 ± 1.8 %) ≈ 0.5 %-Au/Ti3C2 (71 ± 2.8 %) > 1 %-Au/Ti3C2-R (52 ± 5.8 %). The catalytic activity peaks at 0.5 wt% Au loading with reduction pre-treatment and is further enhanced by decreasing the flow rate, benzene concentration, and relative humidity (or by increasing the catalyst mass). The 0.5 %-Au/Ti3C2-R catalyst maintains stable benzene mineralization for 24 h time-on-stream (maximum tested reaction time) at RT without noticeable deactivation. Benzene oxidation on the 0.5 %-Au/Ti3C2-R surface proceeds through diverse reaction intermediates (e.g., phenolate, catecholate, o-, p-benzoquinone, formate, and carbonate). The adsorption of benzene and molecular oxygen (O2) occurs near the Au0 sites. Hydrogen first migrates from benzene to O2, forming an –OOH group attached to Au0. Subsequently, hydrogen transfers from benzene to –OOH, leading to the formation of water as the final product. The benzene ring is then unzipped to yield carbon dioxide through various reaction steps. The present work offers insights into developing Au catalysts for practical DLT control of indoor air pollutants.

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