Li Can, Academician of the Chinese Academy of Sciences, State Key Laboratory of Catalysis Basics, Dalian Academy of Chinese Academy of Sciences, Dr. Li Zelong, Ph.D. student Qu Yuanzhi and others made new progress in the research of CO2 catalytic hydrogenation to produce aromatics Selective conversion to aromatic hydrocarbons. Recently, the research results were published in Joule.
The Li Can team has long been devoted to solar photocatalysis, photoelectric catalysis, electrocatalytic decomposition of water to produce hydrogen and CO2 conversion. The use of clean energy to produce hydrogen to convert CO2 into fuel and chemicals is an important strategy to achieve CO2 emission reduction and sustainable use of carbon resources. Aromatic hydrocarbons are one of the important basic chemical raw materials in the synthesis of organic materials. Aromatic hydrocarbons can be used to synthesize many polymer materials, such as polystyrene, phenol resin, nylon, and polyethylene terephthalate resin. The traditional synthetic methods of aromatic hydrocarbons are mainly the cracking of naphtha and the methanol-to-aromatic hydrocarbon (MTA) pathway developed in recent years based on coal-to-methanol, both of which need to rely on fossil resources (oil and coal). Therefore, the use of renewable energy hydrogen to convert CO2 into aromatic hydrocarbons with high added value, so that CO2 is stored in the form of polymer materials, not only can realize the utilization of CO2 carbon resources, but also can play a role in reducing CO2 emissions, is important Strategic significance. However, CO2 is a thermodynamically inert molecule, and there are great difficulties and challenges in achieving CO2 activation and highly selective conversion.
In this work, Li Can ’s team based on the research of CO2 hydrogenation on ZnZrO solid solution to produce methanol (Science Advances 2017), and the research basis of CO2 hydrogenation on ZnZrO / SAPO series system to produce low-carbon olefins (ACS Catal. 2017) Above, the ZnZrO / ZSM-5 series catalyst system was further constructed. The catalyst converts CO2 hydrogenation into aromatics with high selectivity. When the CO2 conversion rate is 14%, the selectivity of aromatics in hydrocarbons reaches 73% to 78%, while the selectivity of CO can be reduced to 44%. The study found that the key to the hydrogenation of CO2 to aromatic hydrocarbons is the effective synergy of tandem catalysts. Infrared spectroscopy, chemical capture, and experiments show that CO2 and H2 are activated on the ZnZrO solid solution oxide to generate CHxO intermediate species, and the intermediate species migrate from the ZnZrO surface to the molecular sieve pore channel to complete the formation of aromatics. The synergetic mechanism between the tandem catalysts and the surface migration of the key intermediate species CHxO enable the thermodynamic and kinetic coupling of CO2 hydrogenation directly to the aromatic reaction. The appropriate amount of H2O generated in the CO2 hydrogenation reaction can obviously promote the aromatization of olefins by inhibiting the adsorption of weak olefins on the weak acid sites in the molecular sieve. Due to the presence of H2O and CO2 in the reaction system, it provides a weak oxidizing atmosphere, inhibits the formation of polycyclic aromatic hydrocarbons on the catalyst, and extends the life of the catalyst. The catalyst did not show significant deactivation during the 100-hour reaction. This technology expands new ideas for CO2 conversion.
This work was supported by the National Key R & D Program, the National Natural Science Foundation of China and the Strategic Pilot Technology Special Project of the Chinese Academy of Sciences.
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