Xu Zhizhi, Fang Jian, Lu Jichang, He Dedong, He Sufang, Luo Yongming
Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, P. R. China.
Yunnan Research Academy of Eco-environmental Sciences, Kunming 650093, P. R. China.
iScience. 2022 Aug 24;25(9):104999. doi: 10.1016/j.isci.2022.104999. eCollection 2022 Sep 16.
The one-step reaction approach from syngas with hydrogen sulfide (CO/H/HS) over potassium (K) promoted Molybdenum disulfide (MoS) materials can provide alternatives for the synthesis of methanethiol (CHSH). However, the direct confirmation and determination of the real active nature of K-induced 2H and 1T'-MoS for this reaction and the corresponding phase transformation behavior and origin of K-induced 2H-MoS from/to 1T'-MoS remains unclear. Herein, we proved at the atomic level the precise position of K over 1T'-MoS and 2H-MoS species using the technique of HAADF-STEM. A relationship between K-induced 1T' and 2H-MoS phases and the catalytic property to synthesize CHSH was established, and K-intercalated 1T'-MoS phase was confirmed to have excellent catalytic performances. Moreover, the behavior, origin, and influencing factors of phase transformation of 2H-MoS from/to 1T'-MoS in the existence of K were well proved.
在钾(K)促进的二硫化钼(MoS₂)材料上,合成气与硫化氢(CO/H₂/H₂S)一步反应生成甲硫醇(CH₃SH)的方法,可为甲硫醇的合成提供替代方案。然而,对于该反应中K诱导的2H和1T'-MoS₂的实际活性本质,以及K诱导的2H-MoS₂与1T'-MoS₂之间相应的相变行为和起源,仍不清楚。在此,我们利用高角度环形暗场扫描透射电子显微镜(HAADF-STEM)技术,在原子水平上证明了K在1T'-MoS₂和2H-MoS₂物种上的精确位置。建立了K诱导的1T'和2H-MoS₂相之间的关系以及合成CH₃SH的催化性能,并且证实了K插层的1T'-MoS₂相具有优异的催化性能。此外,还很好地证明了在K存在下2H-MoS₂与1T'-MoS₂之间相变的行为、起源和影响因素。