Catalytic CO2 methanation using renewable H2 presents a promising strategy for carbon neutrality and renewable energy storage, yet achieving high efficiency at low temperatures remains a formidable challenge. Herein, we report a Ru/MnO catalyst featuring in situ constructed highly oxyphilic Ru-O-Mn2+ interfaces that demonstrate remarkable CO2 methanation performance. At 180°C and a space velocity of 36,000 mL g-1 h-1, the catalyst achieves 94.9% CO2 conversion with a CH4 production rate of 84.7 µmol gcat -1 s-1, surpassing state-of-the-art catalysts, while maintaining robust stability. Combined experimental and theoretical investigations identify the Ru-O-Mn2+ interface as the pivotal active center, revealing a direct positive correlation between the amount of interfacial oxyphilic species, the quantity of weakly adsorbed CO2, and the turnover frequency. This oxyphilic interfacial site establishes an extensive network for weak CO2 adsorption, thereby promoting CO2 activation at low temperatures. The successful extension of this strategy to Ni-based systems underscores the universality of MnO-mediated interfacial engineering. These findings establish a new design paradigm for low-temperature catalysis and deepen the fundamental understanding of interfacial oxyphilicity in heterogeneous catalysis.
Deng et al. (Wed,) studied this question.