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Plasma-catalytic reforming of CH4-CO2 over porous Ni/N-doped carbon: Efficient syngas production and mechanistic insights
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王
DOI：10.1039/D5CY00936G.png)
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Abstract
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The integration of non-thermal plasma and catalysis offers a promising route for low-temperature reforming of methane (CH4) and carbon dioxide (CO2) into high-value syngas (H2 and CO); enabling efficient activation of stable molecules and tunable product selectivity. However; limitations in energy efficiency; selectivity control; and catalyst dura-bility remain. In this study; a water-cooled dielectric barrier discharge (DBD) reactor cou-pled with a porous nitrogen-doped carbon-supported nickel catalyst (Ni/N–C) was developed to enhance CH4–CO2 reforming performance. The results showed that increasing the CH4/CO2 molar ratio significantly enhanced both reactant conversion and syngas selectivity; while a higher gas flow rate adversely affected conversion efficiency. Under optimal condi-tions (60 mL/min gas flow rate; 1:5 molar ratio of CH4/CO2); CH4 and CO2 conversions reached 44.1% and 20.0%; with CO and H2 selectivities of 67.6% and 48.1%; respectively. The corresponding energy efficiency was 0.39 mmol/kJ. Mechanistic insights derived from catalyst characterization and performance analysis revealed that moderate acid sites pro-moted CH4 activation and facilitated the selective formation of C2 hydrocarbons; while abundant basic sites enhanced CO2 adsorption and activation; thereby improving CO and H2 selectivity. The synergistic effect of acid–base site modulation and plasma-driven activation played a key role in steering the reaction pathway and optimizing product distribution. This work highlighted the potential of tailored Ni-based catalysts for efficient and selective plasma-catalytic reforming of CH4 and CO2 into syngas. Keywords: CH4-CO2 reforming; Non-thermal plasma; Nitrogen-doped carbon; Syngas
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