New progress in research on hydrogenation of carbon dioxide to aromatics

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences Academician Li Can, Ph.D. Li Zelong, Ph.D., Qu Yuanzhi, etc., made new progress in the preparation of aromatic hydrocarbons by catalytic hydrogenation of CO2: direct CO2 is high through the series catalyst system. Selective conversion to aromatics. Recently, the research results were published in Joule.
The Li Can team has long been committed to solar photocatalysis, photocatalysis, electrocatalytic decomposition of water to produce hydrogen and CO2 conversion. The use of clean energy to produce hydrogen to convert CO2 into fuels and chemicals is an important strategy for achieving CO2 emission reduction and sustainable use of carbon resources. Aromatic hydrocarbons are one of the most important basic chemical raw materials in the synthesis of organic materials. Aromatic hydrocarbons can be used to synthesize a variety of polymer materials, such as polystyrene, phenol resin, nylon, and polyethylene terephthalate resin. The synthesis of traditional aromatic hydrocarbons is mainly based on the cracking of naphtha and the methanol-based aromatics (MTA) pathway based on coal-to-methanol in recent years, all of which rely on fossil resources (oil and coal). Therefore, the use of renewable energy hydrogen to convert CO2 into aromatics with high added value, so that CO2 is stored in the form of polymer materials, can achieve CO2 carbon resource utilization, but also play a role in reducing CO2, is important Strategic significance. However, CO2 is a thermodynamically inert molecule, and there are major difficulties and challenges in achieving CO2 activation and high selectivity conversion.
In this work, Li Can's team based on the study of hydrogenation of CO2 on ZnZrO solid solution to produce methanol (Science Advances 2017) and the study of CO2 hydrogenation on ZnZrO/SAPO series system to prepare low-carbon olefins (ACSCatal.2017) Further, a ZnZrO/ZSM-5 series catalyst system was further constructed. The catalyst converts CO2 hydrogenation to aromatics with high selectivity. When the CO2 single pass conversion is 14%, the selectivity of aromatics in hydrocarbons reaches 73% to 78%, and the selectivity of CO can be reduced to 44%. The study found that the key to hydrogenation of CO2 to aromatics is the effective synergy of the series catalysts. Infrared spectroscopy, chemical capture, and experiments show that CO2 and H2 are activated on ZnZrO solid solution oxide to form CHxO intermediate species, and intermediate species migrate from ZnZrO surface to molecular sieve pores to complete the formation of aromatic hydrocarbons. The synergistic mechanism between the series catalysts and the surface migration of the key intermediate species CHxO achieve the thermodynamic and kinetic coupling of the CO2 hydrogenation directly to the aromatics reaction. The proper amount of H2O formed in the CO2 hydrogenation reaction can significantly promote the aromatization of olefins by inhibiting the adsorption of weak olefins in the weak acid sites of the molecular sieves. 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 prolongs the life of the catalyst. The catalyst does not show significant deactivation during the 100 hour reaction. This technology has expanded new ideas for CCO2 conversion.

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