Direct biogas methanation at moderate pressure: Mechanism investigation over Ni-based catalysts

Direct upgrading of biogas by CO2 methanation aims to produce a gas to be injected into the grid. Operating at moderate pressures favors thermodynamics, but catalyst surface and reaction mechanism under realistic conditions are not well investigated. We study the role of basic and metallic sites on...

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Bibliographic Details
Authors: Giarnieri, Ilenia, Chen, Sining, Ballesteros Plata, Daniel, Holgado, Juan P., Maluta, Francesco, Caballero Martínez, Alfonso, Mata Benito, Patricia
Format: article
Status:Published version
Publication Date:2025
Country:España
Institution:Universidad de Sevilla (US)
Repository:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:idus.us.es:11441/173930
Online Access:https://hdl.handle.net/11441/173930
https://doi.org/10.1016/j.jcou.2025.103045
Access Level:Open access
Keyword:Methanation
Hydrotalcite-derived catalyst Nickel
Quasi in situ XPS
In situ DRIFTS
Description
Summary:Direct upgrading of biogas by CO2 methanation aims to produce a gas to be injected into the grid. Operating at moderate pressures favors thermodynamics, but catalyst surface and reaction mechanism under realistic conditions are not well investigated. We study the role of basic and metallic sites on performance and mechanism of clean biogas methanation (CO2/CH4=1/1 v/v) at 1, 5 and 7 bar. Ni/Mg/La/Al hydrotalcite-derived catalysts, with different Ni and La contents, are investigated combining tests and physico-chemical characterization, including quasi-in situ XPS at 7 bar, with CO2-adsorption and methanation DRIFTS at 1 and 7 bar, respectively. An optimized catalyst (6.5 wt% La, 35 wt% Ni) with 3–4 nm Ni0 and balanced basicity, achieves 96 LCH4*gcat− 1 * h− 1 (300◦C, 7 bar). DRIFTS confirm catalysts activity experimental trend. Optimizing Ni and La results in higher consumption rates of formate intermediate and sufficient Ni0 sites for CO formation. Increasing pressure to 7 bar promotes CO and m-HCOO reactivity.