Here, we report a high-performance catalyst MoS x @HSSZ-39 for conversion of CO x to C 2–4 hydrocarbons, in which MoS x clusters for CO x hydrogenation at the first to intermediate methanol and then the zeolitic acid sites surrounding for further conversion of methanol to hydrocarbons. For CO 2 hydrogenation, C 2–4 hydrocarbons of ∼90% selectivity in organic products at 32.7% of CO 2 conversion and excellent stability of 1000 h on stream are obtained. For CO hydrogenation, 95% of C 2–4 hydrocarbons, 83% of LPG or 74% of propane selectivities at > 22% CO conversion and stable more than 200 h on stream are obtained. The cooperation among the MoS x clusters and the zeolitic acid sites constitutes the catalyst of intimate bifunction, which is the key to the high catalytic performance for CO x hydrogenation.
The hydrogenation of CO 2 or CO to single organic product has received widespread attentions. Here we show a highly efficient and selective catalyst, Mo 3 S 4 @ions-ZSM-5, with molybdenum sulfide clusters ([Mo 3 S 4 ] n+ ) confined in zeolitic cages of ZSM-5 molecular sieve for the reactions. Using continuous fixed bed reactor, for CO 2 hydrogenation to methanol, the catalyst Mo 3 S 4 @NaZSM-5 shows methanol selectivity larger than 98% at 10.2% of carbon dioxide conversion at 180 °C and maintains the catalytic performance without any degeneration during continuous reaction of 1000 h. For CO hydrogenation, the catalyst Mo 3 S 4 @HZSM-5 exhibits a selectivity to C 2 and C 3 hydrocarbons stably larger than 98% in organics at 260 °C. The structure of the catalysts and the mechanism of CO x hydrogenation over the catalysts are fully characterized experimentally and theorectically. Based on the results, we envision that the Mo 3 S 4 @ions-ZSM-5 catalysts display the importance of active clusters surrounded by permeable materials as mesocatalysts for discovery of new reactions.
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