Designing main-group catalysts for low-temperature methane combustion by ozone.
Shunsaku YasumuraKenichiro SaitaTakumi MiyakageKen NagaiKenichi KonTakashi ToyaoZen MaenoTetsuya TaketsuguKen-Ichi ShimizuPublished in: Nature communications (2023)
The catalytic combustion of methane at a low temperature is becoming increasingly key to controlling unburned CH 4 emissions from natural gas vehicles and power plants, although the low activity of benchmark platinum-group-metal catalysts hinders its broad application. Based on automated reaction route mapping, we explore main-group elements catalysts containing Si and Al for low-temperature CH 4 combustion with ozone. Computational screening of the active site predicts that strong Brønsted acid sites are promising for methane combustion. We experimentally demonstrate that catalysts containing strong Bronsted acid sites exhibit improved CH 4 conversion at 250 °C, correlating with the theoretical predictions. The main-group catalyst (proton-type beta zeolite) delivered a reaction rate that is 442 times higher than that of a benchmark catalyst (5 wt% Pd-loaded Al 2 O 3 ) at 190 °C and exhibits higher tolerance to steam and SO 2 . Our strategy demonstrates the rational design of earth-abundant catalysts based on automated reaction route mapping.
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