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Investigation of the Active Phase in K-Promoted MoS2 Catalysts for Methanethiol Synthesis
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-01-15 , DOI: 10.1021/acscatal.9b03178 Miao Yu 1 , Nikolay Kosinov 1 , Lennart van Haandel 1 , Patricia J. Kooyman 2 , Emiel J. M. Hensen 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-01-15 , DOI: 10.1021/acscatal.9b03178 Miao Yu 1 , Nikolay Kosinov 1 , Lennart van Haandel 1 , Patricia J. Kooyman 2 , Emiel J. M. Hensen 1
Affiliation
K-promoted MoS2 is an active catalyst for the synthesis of CH3SH, a valuable chemical intermediate, from synthesis gas (CO/H2) and H2S. The promotion of MoS2 by K increases the CO conversion rate and the CH3SH selectivity and is usually linked to the stabilization of the 1T-MoS2 polymorph as compared to the 2H-MoS2 in K-free samples. Sulfided catalysts were characterized using TEM, XPS, and EXAFS. TEM showed that MoS2 particles became larger and more stacked when the K/Mo ratio increased above unity. XPS and EXAFS evidenced the formation of the 1T-MoS2 phase at higher K/Mo ratio in addition to 2H-MoS2. The addition of K to MoS2 led to increased CH3SH productivity due to both increased CO conversion and CH3SH selectivity (T = 300–400 °C, P = 10 bar). The performance of the most active catalyst with a K/Mo ratio of 2 was found to be stable, despite the observation that the initially present 1T-MoS2 phase slowly converted to the 2H-MoS2 phase during the reaction at high pressure. There is no correlation between the CH3SH productivity and the amount of 1T-MoS2 in K-promoted MoS2 catalysts.
中文翻译:
K促进的MoS 2催化合成甲硫醇的活性相的研究
K-促进的MoS 2为CH的合成的活性催化剂3 SH,一个有价值的化学中间体,由合成气(CO / H 2)和H 2 S的促进的MoS的2由k增加CO转化率和与无K样品中的2H-MoS 2相比,CH 3 SH的选择性通常与1T-MoS 2多晶型物的稳定性有关。使用TEM,XPS和EXAFS对硫化催化剂进行了表征。TEM显示,当K / Mo比增加到大于1时,MoS 2颗粒变得更大并且更多地堆叠。XPS和EXAFS证明了1T-MoS 2的形成除了2H-MoS 2以外,还具有较高的K / Mo比。由于增加的CO转化率和CH 3 SH选择性(T = 300–400°C,P = 10 bar),向MoS 2中添加K导致CH 3 SH生产率提高。尽管观察到在高压下反应期间最初存在的1T-MoS 2相缓慢转化为2H-MoS 2相,但是发现K / Mo比为2的最具活性的催化剂的性能稳定。在K促进的MoS 2催化剂中,CH 3 SH生产率与1T-MoS 2的量之间没有相关性。
更新日期:2020-01-15
中文翻译:
K促进的MoS 2催化合成甲硫醇的活性相的研究
K-促进的MoS 2为CH的合成的活性催化剂3 SH,一个有价值的化学中间体,由合成气(CO / H 2)和H 2 S的促进的MoS的2由k增加CO转化率和与无K样品中的2H-MoS 2相比,CH 3 SH的选择性通常与1T-MoS 2多晶型物的稳定性有关。使用TEM,XPS和EXAFS对硫化催化剂进行了表征。TEM显示,当K / Mo比增加到大于1时,MoS 2颗粒变得更大并且更多地堆叠。XPS和EXAFS证明了1T-MoS 2的形成除了2H-MoS 2以外,还具有较高的K / Mo比。由于增加的CO转化率和CH 3 SH选择性(T = 300–400°C,P = 10 bar),向MoS 2中添加K导致CH 3 SH生产率提高。尽管观察到在高压下反应期间最初存在的1T-MoS 2相缓慢转化为2H-MoS 2相,但是发现K / Mo比为2的最具活性的催化剂的性能稳定。在K促进的MoS 2催化剂中,CH 3 SH生产率与1T-MoS 2的量之间没有相关性。