Generating different types of defects in heterogeneous catalysts for synergetic promotion of the reactivity and selectivity in catalytic reactions is highly challenging due to the lack of effective theoretical guidance. Herein, we demonstrate a facile strategy to introduce two types of defects into the CuO-ZnO model catalyst, namely oxygen vacancies (OVs) induced by H₂ partial reduction and localized amorphous regions (LARs) generated via the ball milling process. Using industrially important Rochow–Müller reaction as a representative, we found OVs predominantly improved the target product selectivity of dimethyldichlorosilane, while LARs significantly increased the conversion of reactant Si. The CuO-ZnO catalyst with optimized OVs and LARs contents achieved the best catalytic property. Theoretical calculation further revealed that LARs promote the generation of the Cu₃Si active phase, and OVs impact the electronic structure of the Cu₃Si active phase. This work provides a new understanding of the roles of different catalyst defects and a feasible way of engineering the catalyst structure for better catalytic performances.

Mn-based catalysts have exhibited promising performance in low-temperature selective catalytic reduction of NO_x with NH₃ (NH₃-SCR). However, challenges such as H₂O- or SO₂-induced poisoning to these catalysts still remain. Herein, we report an efficient strategy to prepare the dual single-atom Ce-Ti/MnO₂ catalyst via ball-milling and calcination processes to address these issues. Ce-Ti/MnO₂ showed better catalytic performance with a higher NO conversion and enhanced H₂O- and SO₂-resistance at a low-temperature window (100−150 °C) than the MnO₂, single-atom Ce/MnO₂, and Ti/MnO₂ catalysts. The in situ infrared Fourier transform spectroscopy analysis confirmed there is no competitive adsorption between NO_x and H₂O over the Ce-Ti/MnO₂ catalyst. The calculation results showed that the synergistic interaction of the neighboring Ce-Ti dual atoms as sacrificial sites weakens the ability of the active Mn sites for binding SO₂ and H₂O but enhances their binding to NH₃. The insight obtained in this work deepens the understanding of catalysis for NH₃-SCR. The synthesis strategy developed in this work is easily scaled up to commercialization and applicable to preparing other MnO₂-based single-atom catalysts.