CO2 Methanation in Microstructured Reactors – Catalyst Development and Process Design

• Published in: Chemical engineering & technology 2019-10, Vol.42 (10), p.2076-2084
• Main Authors: Neuberg, Stefan, Pennemann, Helmut, Shanmugam, Vetrivel, Thiermann, Raphael, Zapf, Ralf, Gac, Wojciech, Greluk, Magdalena, Zawadzki, Witold, Kolb, Gunther
• Format: Article
• Language: English
• Subjects: Bimetals; Biogas; Carbon dioxide; Catalysis; Catalyst; Catalysts; Cerium oxides; CO2 methanation; Deactivation; Hydrogen sulfide; Methanation; Microchannels; Microreactors; Power consumption; Reactors; Ruthenium; Sabatier reaction; Selectivity; Silicon dioxide; Stability analysis; Sulfur; Sulfur tolerance; Titanium dioxide
• ISSN: 0930-7516; 1521-4125
• DOI: 10.1002/ceat.201900132

The sulfur tolerance of mono‐ and bimetallic ruthenium catalysts for CO2 hydrogenation was investigated in microchannel reactors. H2S was selected as a model compound. It was found that a Ru/CeO2 catalyst deactivates rapidly. Ni was a much better additive to improve the catalyst stability compared to Rh and serves as a sulfur trap. The influence of the support was evaluated showing that a SiO2‐supported catalyst has a higher stability and better selectivity compared to CeO2 and TiO2. A plant concept was developed comprising two‐step methanation with a first adiabatic reactor stage followed by a plate heat‐exchanger reactor with integrated cooling which allows more than 97 % CO2 conversion. A pilot plant will be put into operation in connection with a biogas plant and an electrolyser of 50 kW power consumption. The sulfur tolerance of ruthenium‐containing catalysts on different supports for CO2 hydrogenation and measures to improve their stability were investigated. A novel plant concept was developed which involves two‐step methanation with a first adiabatic reactor stage followed by a plate heat‐exchanger reactor with integrated cooling that allows for more than 97 % CO2 conversion.