Recently, Sun Jian and Ge Qingjie's research team of the Special Zone for Small Carbon Molecules and Hydrogen Energy Utilization Innovation Special Zone of the Dalian Institute of Chemical Physics, Chinese Academy of Sciences have made new progress in the research of CO2 catalytic hydrogenation to synthesize isoparaffins. Published in the ACS Catalysis published by the Chemical Society.
Using CO2 as a carbon source, and H2 generated from the electrolysis of renewable energy to convert into high value-added hydrocarbons, not only can reduce CO2 emissions, but also solve the problem of excessive dependence on fossil fuels and storage of renewable energy. It has important strategic significance. Precise control of CO bond activation and CC bond coupling is a very challenging problem in CO2 hydroconversion, and is the key to achieving efficient CO2 conversion and utilization. In recent years, the team has realized the direct conversion of CO2 hydrogenation to produce gasoline distillate hydrocarbons (Nature Communications), linear a-olefins (Communications Chemistry) and low-carbon olefins (Catalysis Science & Technology) by designing multi-site catalysts in recent years.
In this work, Wei Jian and Yao Ruwei combined the Na-Fe3O4 and HMCM-22 molecular sieve to form a multi-functional catalyst, and realized the highly efficient cooperative catalysis of three series reactions of reverse water vapor shift, CC coupling and isomerization, and successfully used CO2 and H2 synthesize isoparaffins in one step with high yield. When the conversion rate of CO2 is controlled at about 26%, the CO selectivity is only 17%, the selectivity of C4 + hydrocarbons in hydrocarbons can reach 82%, and the proportion of isoparaffins is as high as 74%, and the space-time yield can reach 105 mgiso gcat-1h-1. Studies have shown that the unique pore structure and Brnsted acid properties of MCM-22 molecular sieve promote the progress of olefin intermediates towards isomerization reaction, while inhibiting aromatization reaction. In addition, the study also discussed the formation process of isoparaffins, the cause of molecular sieve deactivation, the nature of carbon deposit formation, and molecular sieve regeneration methods. This work provides new ideas for the design and application of CO2 hydrogenation to high-carbon hydrocarbon catalysts.
The above research work was supported by the National Natural Science Foundation of China, the Strategic Leading Science and Technology Project of the Chinese Academy of Sciences and the Youth Promotion Association of the Chinese Academy of Sciences.
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