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调整负载型二氧化钛-钯光催化剂中金属-载体相互作用以降解空气中甲苯。

Tuning the metal-support interactions in titanium dioxide-supported palladium photocatalysts against toluene in air.

机构信息

Department of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-ro, Seoul, 04763, Republic of Korea.

Department of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-ro, Seoul, 04763, Republic of Korea.

出版信息

Environ Res. 2024 Dec 15;263(Pt 2):120137. doi: 10.1016/j.envres.2024.120137. Epub 2024 Oct 10.

Abstract

The activity of supported noble metal (e.g., palladium (Pd)) catalysts is often governed by the combined effects of multiple factors (e.g., electronic and geometric properties of the support, surface chemistry of metal nanoparticles (NPs), and metal-support interactions). Pd/titanium dioxide (TiO) catalyst has been developed as a highly efficient photocatalytic degradation (PCD) system against gaseous toluene based on high-temperature pretreatment (300 and 450 °C) in a mixed stream of hydrogen (H) and (N). The interaction of Pd NPs with TiO synergistically improves the PCD efficiency of toluene through the efficient adsorption and activation of toluene as well as molecular oxygen (O) and water (HO) for the facile generation of reactive oxygen species (ROS (e.g., superoxide anion (•O) and hydroxyl (•OH) radicals)). The PCD efficiency of the prepared sample against 5 ppm toluene (at 20% relative humidity (RH)) is 79.6% with the values of maximum reaction rate, quantum yield, space-time yield, and clean air delivery rate as 9.9 μmol g h, 1.68E-03 molecules photon, 1.68E-02 molecules photon g, and 4.8 L h, respectively. Based on this research, the PCD mechanism of gaseous toluene has been explored along with the dynamic behavior of O and HO for ROS generation and their relative contribution to the PCD of toluene. As such, this research offers a perspective for designing advanced photocatalysts through surface defect engineering.

摘要

负载型贵金属(例如钯(Pd))催化剂的活性通常受到多种因素(例如,载体的电子和几何性质、金属纳米粒子(NPs)的表面化学和金属-载体相互作用)的综合影响。Pd/二氧化钛(TiO)催化剂已被开发为一种高效的光催化降解(PCD)系统,可在 H 和(N)的混合气流中,通过高温预处理(300 和 450°C)来有效降解气态甲苯。Pd NPs 与 TiO 的相互作用通过高效吸附和活化甲苯以及分子氧(O)和水(HO),促进了活性氧物种(ROS(例如超氧阴离子(•O)和羟基(•OH)自由基)的生成,从而提高了甲苯的 PCD 效率。所制备样品对 5 ppm 甲苯(在 20%相对湿度(RH)下)的 PCD 效率为 79.6%,最大反应速率、量子产率、时空产率和清洁空气输送率的值分别为 9.9 μmol·g·h、1.68E-03 个分子·光子、1.68E-02 个分子·光子·g 和 4.8 L·h。基于这项研究,探讨了气态甲苯的 PCD 机制,以及 O 和 HO 生成 ROS 的动态行为及其对甲苯 PCD 的相对贡献。因此,这项研究为通过表面缺陷工程设计先进的光催化剂提供了一个视角。

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