Defect‐Engineered Ni@Graphitic Carbon Catalyst With Adaptive Coordination for Energy‐Efficient Plasma‐Assisted Dry Reforming of Methane

Plasma‐assisted dry reforming of methane (DRM) is a promising low‐temperature strategy for syngas production. However, the dynamic and non‐equilibrium nature of the plasma environment presents considerable challenges for catalyst design. Herein, we report a Ni@graphitic carbon catalyst featuring a tailored pore‐surface architecture specifically engineered for plasma‐catalytic conditions. Under ambient temperature and pressure and at a low input power of 40 W, the catalyst achieves remarkable CO and H 2 production rates of 442.56 and 294.4 mmol h −1 g −1 , respectively. The catalyst also maintains stable catalytic performance and structural stability over 100 h of continuous operation, with superior energy efficiency and productivity comparable to state‐of‐the‐art catalysts. Combined theoretical and experimental studies reveal that the unique mesoporous architecture, together with the synergistic coexistence of Ni‐C 4 and Ni‐C/O hetero‐coordination, significantly enhances plasma‐catalytic performance. This work demonstrates that designing plasma‐compatible catalysts with adaptive coordination chemistry provides a powerful route to high‐performance and low‐energy C 1 (one‐carbon) conversion, offering new opportunities for carbon‐neutral syngas production and electrified chemical manufacturing.