figshare
Browse

Unraveling the Promotion Effects of Dynamically Constructed CuO<sub><i>x</i></sub>‑OH Interfacial Sites in the Selective Catalytic Oxidation of Ammonia

Download (2.11 MB)
journal contribution
posted on 2022-03-15, 13:33 authored by Tianwei Lan, Jiang Deng, Xiaoyu Zhang, Fuli Wang, Xiangyu Liu, Danhong Cheng, Dengsong Zhang
The selective catalytic oxidation of ammonia (NH<sub>3</sub>-SCO) into N<sub>2</sub> and H<sub>2</sub>O is a recognized effective protocol to eliminate excessive NH<sub>3</sub> emission. Nevertheless, it is a great challenge for NH<sub>3</sub>-SCO catalysts to balance the NH<sub>3</sub> oxidation activity with N<sub>2</sub> selectivity. Herein, promotion effects of the dynamically constructed CuO<sub><i>x</i></sub>-OH interfacial sites for NH<sub>3</sub> oxidation activity without the scarification of N<sub>2</sub> selectivity were unraveled. The enrichment of coordination unsaturated Cu sites and Cu-OH acid sites in CuO<sub><i>x</i></sub>-OH interfacial sites optimized the adsorption and activation for NH<sub>3</sub> and O<sub>2</sub>, leading to the over 9-fold increase in NH<sub>3</sub> oxidation rate and the 40 kJ/mol decrease in apparent activation energy compared with the conventional CuO sites. Unexpectedly, the fast internal-selective catalytic reduction (i-SCR) mechanism was identified on CuO<sub><i>x</i></sub>-OH interfacial sites, which is characterized by the presence of consumable NO<sub>2</sub> adsorbed species. This work paves an innovative way for the development of effective NH<sub>3</sub>-SCO catalysts and contributes to the deeper understanding of the reaction mechanism.

History