Strong metal-support interaction induced excellent performance for photo-thermal catalysis methane dry reforming over Ru-cluster-ceria catalyst

Abstract

The utilization of solar energy in driving methane dry reforming (MDR) reaction through photo-thermal synergetic catalysis could simultaneously realize the reduction of carbon footprint and the fixation of solar energy, which is an environmentally and economically beneficial route. However, the currently developed catalysts still require further optimization in catalytic performance and stability. Here, we prepared RuNC, a Ru nanoclusters catalyst anchored on CeO₂ with strong metal-support interaction (SMSI) effect via a facile preparation method. The formation rates of H₂ and CO over RuNC catalyst were 1.41 and 2.16 mol·gcat⁻¹·h⁻¹ respectively under photo-thermal catalysis (PTC) at 500 °C, which is up to one order of magnitude higher than existing PTC-MDR catalysts. Moreover, the prepared catalyst did not show significant deactivation under 100 hour test. The in-depth structure-function relationship between catalytic activity/stability and Ru nanocluster sites/induced SMSI effect were determined by systematic structural characterization. The advantages of RuNC catalyst structure under PTC catalytic conditions were demonstrated by optical characterization. Besides, the excitation-migration path of photo-electron under PTC conditions was determined by ISI-XPS experiments. Finally, the mechanism of PTC-MDR reaction and the specific reaction steps enhanced by light irradiation were determined by operando experiments. This work provided theoretical basis and excellent catalyst for the industrial application of PTC-MDR route.