Four Cu/SAPO-34 catalysts are used to research the effect of their acid content on their NH3-SCR activity, by changing the proportion of Si in the catalyst. Though the catalysts exhibit similar Cu loading performed by an ion-exchange method, they lead to different NO conversions in the temperature range of 120–600 °C. The NH3-TPD results show that varying the proportion of Si can adjust the acid content of SAPO-34. In the low temperature range, kinetic tests prove that the various acid contents did not affect the apparent activation energy (Ea) of the Selective Catalytic Reduction by NH3 (NH3-SCR) over Cu/SAPO-34. But it is found that the acid densities are related to the NO conversion at low temperature. In the high temperature range, increasing the acid content of the Cu/SAPO-34 catalysts inhibits the observed NH3 conversions in the NH3 oxidation results. As NH3 oxidation and NH3-SCR are competing reactions and the former can decrease NO conversion, this inhibition is therefore beneficial to NH3-SCR. Finally, the influence of the acid content of the catalysts on the NH3 oxidation is also investigated by kinetic tests.
The process of CH4 cracking into H2 and carbon has gained wide attention for hydrogen production. However, traditional catalysis methods suffer rapid deactivation due to severe carbon deposition. In this study, we discover that effective CH4 cracking can be achieved at 450 °C over a Re/Ni single-atom alloy via ball milling. To explore single-atom alloy catalysis, we construct a library of 10,950 transition metal single-atom alloy surfaces and screen candidates based on C–H dissociation energy barriers predicted by a machine learning model. Experimental validation identifies Ir/Ni and Re/Ni as top performers. Notably, the non-noble metal Re/Ni achieves a hydrogen yield of 10.7 gH2 gcat–1 h–1 with 99.9% selectivity and 7.75% CH4 conversion at 450 °C, 1 atm. Here, we show the mechanical energy boosts CH4 conversion clearly and sustained CH4 cracking over 240 h is achieved, significantly surpassing other approaches in the literature.