CH4 and H2S reforming to CH3SH and H-2 catalyzed by metal-promoted Mo6S8 clusters: a first-principles micro-kinetic study
Journal article, 2017

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.

Methyl Mercaptan

Total-Energy Calculations

Quality Natural-Gas

Augmented-Wave Method

Solid Acid Catalysts

Heterogeneous Catalysis



Molybdenum Sulfide Catalysts

Carbonyl Sulfide



W. Taifan

Lehigh University

Adam Arvidsson

Chalmers, Physics, Chemical Physics

E. Nelson

Lehigh University

Anders Hellman

Chalmers, Physics, Chemical Physics

J. Baltrusaitis

Lehigh University

Catalysis Science and Technology

2044-4753 (ISSN) 2044-4761 (eISSN)

Vol. 7 16 3546-3554

Driving Forces

Sustainable development

Areas of Advance

Nanoscience and Nanotechnology


Materials Science

Subject Categories

Chemical Engineering

Other Physics Topics


C3SE (Chalmers Centre for Computational Science and Engineering)



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4/5/2022 1