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

Taifan William; Arvidsson Adam A.; Nelson EricHellman AndersBaltrusaitis Jonas

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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

机译：甲烷和硫化氢改革CH3SH和,氢催化由metal-promoted Mo6S8集群:一个采用基于micro-kinetic研究

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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.

机译：酸的直接处理,如包含大大量的酸性H2S和/或二氧化碳分子,天然气和大量的直接利益它是可用的和可访问的,但没有得到充分的利用。使用能源密集型胺治疗吸收/解吸,这里我们提出描述一个催化地生产的第一步一个增值化学和能量载体,CH3SH2,分别。密度泛函理论(DFT)和执行microkinetic造型的甲烷和硫化氢反应通路形成CH3SH和2的第一步阐明复杂的但没有探索途径氧酸气改革。我们利用光unpromoted和k或NipromotedMo6S8集群。上面的速率决定步骤1100 KNi-promoted Mo6S8同时,氢是形成在光和K-promoted速率决定步骤Mo6S8。和1100 K, CH3SH形成成为重要的一步,尤其是Ni-Mo6S8。提出了一种有趣的直接催化路线含硫天然气处理潜在的导致高价值的碳氢化合物,如乙烯,使用CH3SH作为反应中间体。

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《Catalysis science & technology》 |2017年第16期|3546-3554|共9页
作者
Taifan William; Arvidsson Adam A.; Nelson EricHellman AndersBaltrusaitis Jonas;
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作者单位

Chalmers, Dept Phys, SE-42196 Gothenburg, Sweden;

Lehigh Univ, Dept Chem & Biomol Engn, B336 Iacocca Hall,111 Res Dr, Bethlehem, PA 18015 USA;

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direct processing; Natural Gas; gas naturaldeuteriumReformingmethaneFirst Stepreaction temperaturedensity functional theoryrate determining step;

机译：直接加工;天然气;气体Stepreaction temperaturedensity功能theoryrate确定步骤;

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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

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