| Popis: |
The catalytic combustion of methane (CH4) at a low temperature is becoming increasingly key to controlling unburned CH4 emissions from natural gas vehicles and power plants, although the low activity of benchmark platinum-group-metal (PGM) catalysts hinders its application. Based on the automated reaction route mapping, we designed the main-group catalyst for low-temperature CH4 combustion with ozone (O3). The computational screening of the active site predicted the strong Brønsted acid sites (BASs) as promising ones. We experimentally demonstrated that the catalyst comprising strong BASs exhibited improved CH4 conversion at 200 °C, correlating with the theoretically predicted design concept. The main-group catalyst (proton-type beta zeolite) delivered a reaction rate, which was 442 times higher than that of a benchmark catalyst (5wt% Pd-loaded Al2O3), at 190 °C and exhibited higher tolerance to steam and SO2. Our strategy demonstrated the rational design of earth-abundant catalysts based on automated reaction route mapping. |
