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CH4 and H2S reforming to CH3SH and H-2 catalyzed by metal-promoted Mo6S8 clusters: a first-principles micro-kinetic study

W. Taifan ; Adam Arvidsson (Institutionen för fysik, Kemisk fysik (Chalmers)) ; E. Nelson ; Anders Hellman (Institutionen för fysik, Kemisk fysik (Chalmers)) ; J. Baltrusaitis
Catalysis Science & Technology (2044-4753). Vol. 7 (2017), 16, p. 3546-3554.
[Artikel, refereegranskad vetenskaplig]

Direct processing of sour, e.g. containing large amounts of acidic H2S and/or CO2 molecules, natural gas is of direct interest as vast amounts of it are available and accessible but are underutilized. While sour natural gas is still treated using energy-intensive amine absorption/desorption, here we propose and describe a first step in catalytically producing a value added chemical and energy carrier, CH3SH and H-2, respectively. For this purpose, we performed Density Functional Theory (DFT) and microkinetic modelling of CH4 and H2S reaction pathways to form CH3SH and H-2 as a first step in elucidating complex yet not explored pathways in oxygen-free sour gas reforming. For this purpose, we utilized bare unpromoted and K-or Nipromoted Mo6S8 clusters. CH4 dissociation was found to be the rate-determining step above 1100 K on Ni-promoted Mo6S8 while H-2 formation was the rate-determining step on the bare and K-promoted Mo6S8. At lower reaction temperatures between 800 and 1100 K, CH3SH formation becomes an important step, especially on Ni-Mo6S8. This method presents an interesting route of direct catalytic sour natural gas processing which potentially leads to high-value hydrocarbons, such as ethylene, using CH3SH as a reactive intermediate.

Nyckelord: Solid Acid Catalysts, Molybdenum Sulfide Catalysts, Initio, Molecular-Dynamics, Total-Energy Calculations, Augmented-Wave Method, Quality Natural-Gas, Hydrogen-Production, Methyl Mercaptan, Heterogeneous Catalysis, Carbonyl Sulfide

Denna post skapades 2017-09-05.
CPL Pubid: 251634


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