Amorphous Nanoconfinement Enables Self-sustaining Sabatier Reaction at Ambient Conditions

Abstract

The Sabatier reaction, the catalytic hydrogenation of CO2 into CH4, offers a cornerstone for carbon capture and utilization, and in-situ resource utilization during space exploration; however, it faces a fundamental thermodynamic-kinetic paradox: although highly exothermic, conventional catalysts still require continuous external heating to activate CO2 and maintain stable operation. Here we report an amorphous silica-embedded ruthenium catalyst that enables a long-term self-sustaining autothermal Sabatier reaction dispensing with external energy supply. Operating under ambient conditions, this system achieves a record-high CH4 yield of 0.50 mol gcat-1 h-1 with 100% selectivity, stable operation for over 2,000 hours, and a record-low catalyst bed temperature down to 100 oC. This exceptional self-sustaining behavior stems from the synergistic effect of the catalyst's ultralow effective thermal conductivity (0.27 W m-1 K-1), induced by amorphous nanoconfinement, and its superior intrinsic activity. This synergy generates localized hot spots at Ru sites while suppressing macroscopic heat loss. In situ measurements further reveal CH4 formation even at 54 oC and identify a *CO-mediated pathway for CO2 methanation. The reaction ignites readily with a lighter or focused sunlight and persists even under forced convection from an electric fan, demonstrating strong environmental tolerance. By removing the need for constant energy input, this "ignite-and-forget" system paves the way for decentralized Power-to-Gas systems and autonomous fuel production in resource-constrained environments like Mars.