Abstract

Dry reforming of methane (DRM) enables the resource utilization of greenhouse gases, yet conventional thermal catalysis is limited by excessive energy input and serious carbon coking deactivation. Herein, we propose a non-thermal catalytic strategy integrating dielectric barrier discharge (DBD) low-temperature plasma with Ni single-atom catalysts. A hierarchical NiFe/3D NC single-atom catalyst with Ni-N₂ low-coordination configuration, Fe promoter doping and 3D porous carbon matrix was synthesized by the template-assisted hydrothermal-calcination method. Significant synergy occurs between plasma-generated high-energy electrons and unsaturated single-atom sites, which greatly reduces the apparent activation energy. At optimized discharge conditions, CH₄ and CO₂ conversions attain 94.03% and 75.57%, respectively. The reversible Fe²⁺/Fe³⁺ redox cycle removes surface dissociated carbon species and sustains long-term catalytic stability. This work clarifies the dynamic interaction mechanism between plasma field and hierarchical single-atom catalysts and offers theoretical basis for carbon energy conversion under mild environments.