Li Zhuocan, Duan Rucheng, Wang Xin, Fu Yu, Gao Meng, Li Hongwei, He Guangzhi, He Hong
State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, 100085, China.
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2025 Jul 7;64(28):e202501957. doi: 10.1002/anie.202501957. Epub 2025 May 19.
Promoters can greatly improve the activity of catalysts; however, the mechanism by which they interact with the primary catalyst to enhance catalytic activity is not always clear. It has been widely demonstrated that WO in VO-WO/TiO catalysts acts as a promoter to enhance the surface acidity and regulate the dispersion of active VO species, while it is believed that the redox process takes place entirely at the V sites in the selective catalytic reduction of NO with NH (NH-SCR). Here, by combining in situ spectroscopic measurements and density functional theory (DFT) calculations, we validate that the WO directly participates in the oxidative activation of NH, and hence explicitly exerts a redox effect in NH-SCR by forming V-W dinuclear sites with VO. This study sheds new light on a long-standing puzzle regarding the role of WO as a promoter and hence advances the understanding of the working principle of VO-WO/TiO catalysts.
助催化剂能够极大地提高催化剂的活性；然而，它们与主催化剂相互作用以增强催化活性的机制并不总是清晰的。已有广泛研究表明，在VO-WO/TiO催化剂中，WO作为助催化剂可增强表面酸性并调节活性VO物种的分散，而人们认为在以NH选择性催化还原NO（NH-SCR）过程中，氧化还原过程完全发生在V位点上。在此，通过结合原位光谱测量和密度泛函理论（DFT）计算，我们证实WO直接参与NH的氧化活化，因此通过与VO形成V-W双核位点在NH-SCR中明确发挥氧化还原作用。这项研究为长期以来关于WO作为助催化剂的作用这一谜题提供了新的线索，从而推动了对VO-WO/TiO催化剂工作原理的理解。
