Plasma‐Driven Fe/Cu‐MOF Catalyzed CO ₂ Decomposition to CO

Room‐temperature plasma‐assisted catalysis represents an important pathway for CO 2 valorization. Rational design of catalysts tailored to plasma environment holds significant potential for improving catalytic efficiency. Unprecedentedly, we report a coordination‐engineering strategy to fabricate the Fe/Cu mix‐metal organic framework (Fe/Cu‐MOF) catalysts for plasma‐driven CO 2 dissociation into CO. Precise modulation during synthesis revealed an optimal Fe:Cu ratio of 0.44:0.56 to generating synergistic active sites favorable for CO production. The in situ‐formed FeCu‐based catalyst exhibited exceptionally high CO space‐time yield of 32.3 mmol·gcat‐1·h‐1 under room‐temperature plasma conditions. The coordination‐tailored electronic structure enables the dynamic variations in the oxidation states of Fe/Cu upon plasma activation, thus facilitating sustained CO 2 activation. This work establishes atomic‐level control of bimetallic sites as a powerful paradigm for plasma‐catalytic systems.