Ni/ZrO₂ Catalysts Synthesized via Urea Combustion Method for CO₂ Methanation

Abstract

A series of Ni/ZrO₂ catalysts were synthesized by urea combustion method for CO₂ 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/ZrO₂–O catalyst derived from zirconium oxynitrate hydrate exhibited better catalytic activity than the Ni/ZrO₂ 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/ZrO₂–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% CO₂ conversion and 100% CH₄ selectivity at 300 °C, 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 ZrO₂ to tetragonal ZrO₂ accompanied by the incorporation of oxygen vacancies in the ZrO₂ lattice. This phenomenon can also be related to the high catalytic activity of the as-prepared catalysts.

Keywords

Urea combustion method / Nickel / CO₂ methanation / Zirconium precursor / Urea / ZrO₂

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