Investigation of sulfur-resistant, highly active unsupported MoS2 catalysts for synthetic natural gas production from CO methanation
Investigation of sulfur-resistant, highly active unsupported MoS2 catalysts for synthetic natural gas production from CO methanation
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DOI：
10.1016/j.fuproc.2013.01.003
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发表时间：
2013-06
影响因子：
7.5
通讯作者：
Jia Liu;E. Wang;Jing Lv;Zhenhua Li;Baowei Wang;Xinbin Ma;Shaodong Qin;Qi Sun
中科院分区：
文献类型：
--
作者：
Jia Liu;E. Wang;Jing Lv;Zhenhua Li;Baowei Wang;Xinbin Ma;Shaodong Qin;Qi Sun
本文报道了通过在催化剂制备中引入硫粉代替有毒的H2S来提高耐硫甲烷化催化剂的活性。考虑到经济性和活性，七钼酸铵（AHM）是制备该催化剂的合适前体。研究了S/AHM重量比和硫化气氛对催化剂甲烷化性能的影响，最佳S/AHM比为3。硫化气氛不仅影响甲烷化活性，还影响催化剂的结构和形貌。惰性气氛处理的催化剂表现出相对最高的甲烷化活性，CO转化率高达88.2%，接近热力学平衡值。催化剂表征结果表明，S/AHM比为3时所制备的催化剂比其他S/AHM比的催化剂具有较高的比表面积和较大的孔体积。 MoS2颗粒结晶不良，呈长而直的多层板状。对于在氮气环境下处理的催化剂，表面存在更多的弱键合硫物种，并且MoS2颗粒的边缘平面存在更多的硫空位，这些空位被认为是甲烷化的活性位点。
This paper reports on an enhanced activity of sulfur-resistant methanation catalyst by introducing sulfur powder instead of toxic H2S in catalyst preparation. Ammonium heptamolybdate (AHM) was a suitable precursor for this catalyst preparation based on consideration of economy and activity. The effect of S/AHM weight ratio and sulfidation atmosphere on catalyst methanation performance was studied and the optimum S/AHM ratio was 3. Sulfidation atmosphere affected not only methanation activity but also the structure and morphology of the catalysts. The catalyst treated in inert atmosphere exhibited relatively the highest methanation activity with CO conversion as high as 88.2%, which was approaching the thermodynamic equilibrium value. The catalysts characterization results indicated that the as-prepared catalyst at S/AHM ratio as 3 had relatively higher specific surface area and larger pore volume than those with other S/AHM ratio. The MoS2particles were poorly crystallized with long and straight multi-layered slabs. For the catalyst treated in nitrogen environment, more weakly-bonded sulfur species existed on the surface and more sulfur vacancies resided on the edge planes of MoS2particles, which are considered to be the active sites for methanation.