CNT and H2 Production During CH4 Decomposition over Ni/CeZrO2. I. A Mechanistic Study

This work presents a new insight into the potential of a Ni/CeZrO2 catalyst in two separate processes: (i) Chemical Vapor Deposition (CVD) using methane as a feedstock to obtain carbon nanotubes (CNTs) and H2, and (ii) catalyst regeneration with H2O that yields H2. The direct reaction of methane with H2O (steam methane reforming (SMR)) leads to H2 and CO (and CO2), whereas carbon deposition—regardless of its type—is an unwanted reaction. The concept presented in this work assumes dividing that process into two reactors, which allows one to obtain two valuable products, i.e., CNTs and H2. The literature data on CNT production via CVD ignores the issue of H2 formation. Moreover, there is no data concerning CNT production in fluidized bed reactors over ceria-zirconia supported metal catalysts. The results presented in this work show that CNTs can be formed on Ni/CeZrO2 during CH4 decomposition, and that the catalyst can be easily regenerated with H2O, which is accompanied by a high production of H2. The ability of Ni/CeZrO2 to be regenerated is its main advantage over the Ni-MgO catalyst that is popular for CNT production. This paper also shows that the Ni/CeZrO2 catalyst has the potential to be used for CNT and H2 production in a larger scale process, e.g., in a fluidized bed reactor