Single-atom catalysts reveal the dinuclear characteristic of active sites in NO selective reduction with NH(3)

单原子催化剂揭示了 NH(3) 选择性还原 NO 中活性位点的双核特征

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Abstract

High-performance catalysts are extremely required for controlling NO emission via selective catalytic reduction (SCR), and to acquire a common structural feature of catalytic sites is one key prerequisite for developing such catalysts. We design a single-atom catalyst system and achieve a generic characteristic of highly active SCR catalytic sites. A single-atom Mo(1)/Fe(2)O(3) catalyst is developed by anchoring single acidic Mo ions on (001) surfaces of reducible α-Fe(2)O(3), and the individual Mo ion and one neighboring Fe ion are thus constructed as one dinuclear site. As the number of the dinuclear sites increases, SCR rates increase linearly but the apparent activation energy remains almost unchanged, evidencing the identity of the dinuclear active sites. We further design W(1)/Fe(2)O(3) and Fe(1)/WO(3) and find that tuning acid or/and redox properties of dinuclear sites can alter SCR rates. Therefore, this work provides a design strategy for developing improved SCR catalysts via optimizing acid-redox properties of dinuclear sites.

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