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COx hydrogenation to methanol and other hydrocarbons under mild conditions with Mo3S4@ZSM-5
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COx hydrogenation to methanol and other hydrocarbons under mild conditions with Mo3S4@ZSM-5
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Journal Article
COx hydrogenation to methanol and other hydrocarbons under mild conditions with Mo3S4@ZSM-5
2023
Overview
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.
A series of materials containing Mo-S clusters confined in zeolitic cages of ZSM-5 are reported and shown to be efficient for CO
2
or CO hydrogenation with >98% selectivity to methanol, stable over 1000 h, or C
2
and C
3
hydrocarbons, stable over 100 h.
