摘要
A series of Ni/ZrO_2 catalysts were synthesized by urea combustion method for CO_2 methanation.The effects of zirconium precursors and urea dosage on the structure and catalytic performance of the catalysts were tested.Results showed that the Ni/ZrO_2–O catalyst derived from zirconium oxynitrate hydrate exhibited better catalytic activity than the Ni/ZrO_2 catalyst because of its higher Ni dispersion and smaller Ni particle size.In addition,the urea dosage significantly influenced the low-temperature activity of the catalysts by affecting the metal–support interaction,Ni dispersion,and Ni particle size.The Ni/ZrO_2–O-0.4 catalyst with a urea-to-nitrate molar ratio of 0.4 exhibited the best catalytic activity owing to its moderate metal–support interaction,highest Ni dispersion,and smallest Ni particle size,achieving 69.2% CO_2 conversion and 100% CH_4 selectivity at 300℃,0.1 MPa,and a weight hour space velocity(WHSV)of 50,000 mL/(g·h).Moreover,the urea combustion method can lead to the entire phase transformation from monoclinic ZrO_2 to tetragonal ZrO_2 accompanied by the incorporation of oxygen vacancies in the ZrO_2 lattice.This phenomenon can also be related to the high catalytic activity of the as-prepared catalysts.
A series of Ni/ZrO_2 catalysts were synthesized by urea combustion method for CO_2 methanation.The effects of zirconium precursors and urea dosage on the structure and catalytic performance of the catalysts were tested.Results showed that the Ni/ZrO_2–O catalyst derived from zirconium oxynitrate hydrate exhibited better catalytic activity than the Ni/ZrO_2 catalyst because of its higher Ni dispersion and smaller Ni particle size.In addition,the urea dosage significantly influenced the low-temperature activity of the catalysts by affecting the metal–support interaction,Ni dispersion,and Ni particle size.The Ni/ZrO_2–O-0.4 catalyst with a urea-to-nitrate molar ratio of 0.4 exhibited the best catalytic activity owing to its moderate metal–support interaction,highest Ni dispersion,and smallest Ni particle size,achieving 69.2% CO_2 conversion and 100% CH_4 selectivity at 300℃,0.1 MPa,and a weight hour space velocity(WHSV)of 50,000 mL/(g·h).Moreover,the urea combustion method can lead to the entire phase transformation from monoclinic ZrO_2 to tetragonal ZrO_2 accompanied by the incorporation of oxygen vacancies in the ZrO_2 lattice.This phenomenon can also be related to the high catalytic activity of the as-prepared catalysts.
