COx hydrogenation to methanol and other hydrocarbons under mild conditions with Mo3S4@ZSM-5

Gui Liu, Pengfei Liu, Deming Meng, Taotao Zhao, Xiaofeng Qian, Qiang He, Xuefeng Guo, Jizhen Qi, Luming Peng, Nianhua Xue, Yan Zhu, Jingyuan Ma (), Qiang Wang (), Xi Liu (), Liwei Chen and Weiping Ding ()
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Gui Liu: Nanjing University
Pengfei Liu: Nanjing Tech University
Deming Meng: Nanjing University
Taotao Zhao: Nanjing University
Xiaofeng Qian: Nanjing University
Qiang He: Nanjing University
Xuefeng Guo: Nanjing University
Jizhen Qi: Chinese Academy of Sciences
Luming Peng: Nanjing University
Nianhua Xue: Nanjing University
Yan Zhu: Nanjing University
Jingyuan Ma: Pudong New District
Qiang Wang: Nanjing Tech University
Xi Liu: Shanghai Jiao Tong University
Liwei Chen: Chinese Academy of Sciences
Weiping Ding: Nanjing University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract The hydrogenation of CO2 or CO to single organic product has received widespread attentions. Here we show a highly efficient and selective catalyst, Mo3S4@ions-ZSM-5, with molybdenum sulfide clusters ([Mo3S4]n+) confined in zeolitic cages of ZSM-5 molecular sieve for the reactions. Using continuous fixed bed reactor, for CO2 hydrogenation to methanol, the catalyst Mo3S4@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 Mo3S4@HZSM-5 exhibits a selectivity to C2 and C3 hydrocarbons stably larger than 98% in organics at 260 °C. The structure of the catalysts and the mechanism of COx hydrogenation over the catalysts are fully characterized experimentally and theorectically. Based on the results, we envision that the Mo3S4@ions-ZSM-5 catalysts display the importance of active clusters surrounded by permeable materials as mesocatalysts for discovery of new reactions.

Date: 2023
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DOI: 10.1038/s41467-023-36259-9

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