Watanabe Ryo, Oba Natsu, Smith Suchada, Oshima Kazumasa, Kishida Masahiro, Miyake Koji, Nishiyama Norikazu, Verma Priyanka, Fukuhara Choji
Department of Applied Chemistry and Biochemical Engineering, Graduate School of Engineering, Shizuoka University 3-5-1 Johoku, Naka-ku, Hamamatsu Shizuoka 432-8561 Japan
Department of Chemical Engineering, Faculty of Engineering, Kyushu University 744 Motooka Nishi-ku, Fukuoka-shi Fukuoka 819-0395 Japan.
RSC Adv. 2023 Jul 18;13(31):21441-21447. doi: 10.1039/d3ra01852k. eCollection 2023 Jul 12.
The catalytic properties of conventional H-[Al]-ZSM-5 and gallium-substituted H-[Ga]-ZSM-5 were evaluated in the conversion of methanethiol to ethylene (CHSH → 1/2CH + HS). Dimethyl sulfide (DMS), aromatics, and CH were formed as byproducts on the H-[Al]-ZSM-5 catalyst. The introduction of Ga into the ZSM-5 structure provided a high ethylene yield with relatively high selectivity for olefins. Based on the temperature-programmed desorption of NH and pyridine adsorption on zeolites, the strength of acid sites was decreased by introducing Ga into the ZSM-5 structure. Undesirable reactions seemed less likely to occur at weakly acidic sites. The suppression of the formation of dimethyl sulfide (CHSH → 1/2CHS + 1/2HS) and the sequential reaction of ethylene to produce aromatics provided a high yield of ethylene over H-[Ga]-ZSM-5.
在甲硫醇转化为乙烯（CH₃SH → 1/2C₂H₄ + H₂S）的反应中，对传统的H-[Al]-ZSM-5和镓取代的H-[Ga]-ZSM-5的催化性能进行了评估。在H-[Al]-ZSM-5催化剂上，副产物有二甲硫醚（DMS）、芳烃和C₂H₄。将Ga引入ZSM-5结构中，可实现较高的乙烯产率，并对烯烃具有较高的选择性。基于NH₃程序升温脱附和吡啶在沸石上的吸附，将Ga引入ZSM-5结构会降低酸位点的强度。在弱酸性位点上，不良反应似乎不太可能发生。抑制二甲硫醚的形成（CH₃SH → 1/2C₂H₆S + 1/2H₂S）以及乙烯生成芳烃的后续反应，使得H-[Ga]-ZSM-5具有较高的乙烯产率。
