Oxyphilic Ru‐O‐Mn 2+ Interfaces on Ru/MnO Catalysts: Unprecedented Activity for Low‐Temperature CO 2 Methanation

ABSTRACT Catalytic CO 2 methanation using renewable H 2 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–Mn 2+ interfaces that demonstrate remarkable CO 2 methanation performance. At 180°C and a space velocity of 36,000 mL g −1 h −1 , the catalyst achieves 94.9% CO 2 conversion with a CH 4 production rate of 84.7 µmol g cat −1 s −1 , surpassing state‐of‐the‐art catalysts, while maintaining robust stability. Combined experimental and theoretical investigations identify the Ru–O–Mn 2+ interface as the pivotal active center, revealing a direct positive correlation between the amount of interfacial oxyphilic species, the quantity of weakly adsorbed CO 2 , and the turnover frequency. This oxyphilic interfacial site establishes an extensive network for weak CO 2 adsorption, thereby promoting CO 2 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.