Ni/La-γ-Al 2 O 3 samples containing 13.6 wt.% Ni and a variable amount of lanthana (0, 4, 14 and 37 wt.%) were prepared by incipient wetness impregnation, using silica-free γ-Al 2 O 3 support. The materials were characterized, as such or after reaction, with XRD, H 2 -TPR, IR, UV–vis-NIR, XPS and FE-SEM techniques. They were tested as catalysts for CO 2 methanation at atmospheric pressure at GHSV 55000 h −1 . The reaction is under kinetic control at T < 650–673 K, while the product mixture is under thermodynamic control above this temperature range. Lanthanum addition strongly increases the activity of Ni/γ-Al 2 O 3 for CO 2 methanation. Methane selectivity is increased to nearly 100% at low temperatures (T < 650 K). The CO 2 methanation reaction on La-doped Ni/γ-Al 2 O 3 occurs with similar activation energies (80 kJ/mol), and with slightly higher reaction order for hydrogen and lower reaction order for CO 2 than those observed for undoped Ni/γ-Al 2 O 3 . Lanthanum acts as a promoter because of the stronger basicity of the lanthana-alumina support allowing stronger adsorption of CO 2 as surface carbonates that can be act as “reactant reservoirs”. The Ni/La-alumina catalysts studied here are similarly effective as Ru/alumina catalysts for the selective CO 2 methanation at low temperature and atmospheric pressure.

A study of Ni/La-Al 2 O 3 catalysts: A competitive system for CO 2 methanation

Garbarino, Gabriella;Cavattoni, Tullio;Finocchio, Elisabetta;Riani, Paola;Busca, Guido
2019-01-01

Abstract

Ni/La-γ-Al 2 O 3 samples containing 13.6 wt.% Ni and a variable amount of lanthana (0, 4, 14 and 37 wt.%) were prepared by incipient wetness impregnation, using silica-free γ-Al 2 O 3 support. The materials were characterized, as such or after reaction, with XRD, H 2 -TPR, IR, UV–vis-NIR, XPS and FE-SEM techniques. They were tested as catalysts for CO 2 methanation at atmospheric pressure at GHSV 55000 h −1 . The reaction is under kinetic control at T < 650–673 K, while the product mixture is under thermodynamic control above this temperature range. Lanthanum addition strongly increases the activity of Ni/γ-Al 2 O 3 for CO 2 methanation. Methane selectivity is increased to nearly 100% at low temperatures (T < 650 K). The CO 2 methanation reaction on La-doped Ni/γ-Al 2 O 3 occurs with similar activation energies (80 kJ/mol), and with slightly higher reaction order for hydrogen and lower reaction order for CO 2 than those observed for undoped Ni/γ-Al 2 O 3 . Lanthanum acts as a promoter because of the stronger basicity of the lanthana-alumina support allowing stronger adsorption of CO 2 as surface carbonates that can be act as “reactant reservoirs”. The Ni/La-alumina catalysts studied here are similarly effective as Ru/alumina catalysts for the selective CO 2 methanation at low temperature and atmospheric pressure.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11567/942328
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