Liao Yujie, Zhao Kun, Chen Ke, Sun Chenghua, Fu Dong
Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, P. R. China.
MOE Key Laboratory of Resources and Environmental Systems Optimization, North China Electric Power University, Beijing 102206, P. R. China.
ACS Omega. 2023 Jul 12;8(29):26045-26054. doi: 10.1021/acsomega.3c02132. eCollection 2023 Jul 25.
For environmental catalysis, a central topic is the design of high-performance catalysts and advanced mechanism studies. In the case of the removal of flue gas pollutants from coal-fired power plants, highly selective nanoreactors have been widely utilized together with plasma discharge characteristics, such as the catalytic oxidation of NO. Herein, a novel reactor with a three-dimensional hollow structure of TiO confining CoO nanoclusters (CoO/TiO-3DHS) has been developed for plasma-catalytic oxidation of NO, whose performance was compared with that of the commercial TiO confining CoO cluster (CoO/TiO). Specifically, CoO/TiO-3DHS presented a higher efficiency (almost 100%) within lower peak-peak voltage (). More importantly, the NO oxidation efficiency was between 91.5 and 94.5% after a long time of testing, indicating that CoO/TiO-3DHS exhibits more robust sulfur and water tolerance. Density functional theory calculations revealed that such impressive performance originates from the unique cluster-support effect, which changes the distribution of the active sites on the catalyst surface, resulting in the selective adsorption of flue gas. This investigation provides a new strategy for constructing a three-dimensional hollow nanoreactor for the plasma-catalytic process.
对于环境催化而言，一个核心主题是高性能催化剂的设计和深入的机理研究。在去除燃煤电厂烟气污染物的情况下，高选择性纳米反应器已与等离子体放电特性一起被广泛应用，例如NO的催化氧化。在此，已开发出一种具有TiO三维中空结构且限域CoO纳米团簇的新型反应器（CoO/TiO-3DHS）用于NO的等离子体催化氧化，并将其性能与商业TiO限域CoO团簇（CoO/TiO）的性能进行了比较。具体而言，CoO/TiO-3DHS在较低的峰-峰值电压下表现出更高的效率（几乎100%）。更重要的是，经过长时间测试后，NO氧化效率在91.5%至94.5%之间，这表明CoO/TiO-3DHS表现出更强的耐硫和耐水性能。密度泛函理论计算表明，这种令人印象深刻的性能源于独特的团簇-载体效应；该效应改变了催化剂表面活性位点的分布，从而导致对烟气的选择性吸附。本研究为构建用于等离子体催化过程的三维中空纳米反应器提供了一种新策略。
