CO_(2) methanation using nickel-based catalysts has attracted large interest as a promising power-to-gas route.Ni nanoparticles supported on nitrogen-doped CNTs with Ni loadings in the range from 10 wt% to 50 wt% were...CO_(2) methanation using nickel-based catalysts has attracted large interest as a promising power-to-gas route.Ni nanoparticles supported on nitrogen-doped CNTs with Ni loadings in the range from 10 wt% to 50 wt% were synthesized by impregnation,calcination and reduction and characterized by elemental analysis,X-ray powder diffraction,H_(2) temperature-programmed reduction,CO pulse chemisorption and transmission electron microscopy.The Ni/NCNT catalysts were highly active in CO_(2) methanation at atmospheric pressure,reaching over 50% CO_(2) conversion and over 95% CH_(4) selectivity at 340℃ and a GHSV of50,000 mL g^(-1) h^(-1) under kinetically controlled conditions.The small Ni particle sizes below 10 nm despite the high Ni loading is ascribed to the efficient anchoring on the N-doped CNTs.The optimum loading of 30 wt%-40 wt% Ni was found to result in the highest Ni surface area,the highest degree of conversion and the highest selectivity to methane.A constant TOF of 0.3 s^(-1) was obtained indicating similar catalytic properties of the Ni nanoparticles in the range from 10 wt%to 50 wt% Ni loading.Long-term experiments showed that the Ni/NCNT catalyst with 30 wt% Ni was highly stable for 100 h time on stream.展开更多
基金supported by the Ministry of Economic Affairs,Innovation,Digitalization and Energy of the State of North Rhine-Westphalia,W041A。
文摘CO_(2) methanation using nickel-based catalysts has attracted large interest as a promising power-to-gas route.Ni nanoparticles supported on nitrogen-doped CNTs with Ni loadings in the range from 10 wt% to 50 wt% were synthesized by impregnation,calcination and reduction and characterized by elemental analysis,X-ray powder diffraction,H_(2) temperature-programmed reduction,CO pulse chemisorption and transmission electron microscopy.The Ni/NCNT catalysts were highly active in CO_(2) methanation at atmospheric pressure,reaching over 50% CO_(2) conversion and over 95% CH_(4) selectivity at 340℃ and a GHSV of50,000 mL g^(-1) h^(-1) under kinetically controlled conditions.The small Ni particle sizes below 10 nm despite the high Ni loading is ascribed to the efficient anchoring on the N-doped CNTs.The optimum loading of 30 wt%-40 wt% Ni was found to result in the highest Ni surface area,the highest degree of conversion and the highest selectivity to methane.A constant TOF of 0.3 s^(-1) was obtained indicating similar catalytic properties of the Ni nanoparticles in the range from 10 wt%to 50 wt% Ni loading.Long-term experiments showed that the Ni/NCNT catalyst with 30 wt% Ni was highly stable for 100 h time on stream.