Nickel and Nitrogen Co-doped Biomass Carbon-based Catalysts Used for the Electrochemical Reduction of CO2 to Prepare Syngas
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Graphical Abstract
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Abstract
To address CO2 emissions caused by excessive fossil fuel consumption, a novel Ni-N co-doped biomass-derived carbon catalyst (Ni-NBC-800) is developed using agricultural waste corn stalks, aiming to achieve electrochemical CO2 reduction (CO2 Reduction Reaction, CO2RR) for synthesizing syngas (CO/H2) with tunable ratios and promote CO2 resource utilization. A NH4Cl-assisted pore-forming strategy combined with nickel impregnation and high-temperature pyrolysis is employed to construct a composite catalyst featuring hierarchical porous structures and metal-nitrogen active sites. Experimental results demonstrate that with the optimized mass fraction of the load Ni (2%) and calcination temperature (800 ℃), the catalyst achieved a CO Faradaic efficiency of 72.8% at –0.8 V, while the molar ratio of CO to H2 can be continuously adjusted within the range of 0.75 to 3.15 through potential regulation, meeting downstream syngas process requirements. Compared with commercial activated carbon-based catalyst (Ni-NAC-800), Ni-NBC-800 exhibited superior CO partial current density (–4.75 mA/cm2) and stability (the 24-hour current retention rate of 90.3%). Characterization analyses revealed that the hierarchical porous structure formed by NH3/HCl gas synergistic etching during NH4Cl pyrolysis significantly enhanced reactant mass transfer and catalytic activity. This work not only validates the feasibility of agricultural waste-derived carbon materials as alternatives to commercial carbon supports, but also provides a new strategy for low-cost and tunable syngas electrosynthesis through metal-support synergistic design.
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