1. Engineering Research Center of Large-Scale Reactor Engineering and Technology, Ministry of Education, East China University of Science and Technology, Shanghai 200237, China 2. Department of Product Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
Alkylation of benzene to value-added, high octane number and low toxic toluene and xylenes provides a way to lower benzene content in gasoline pool, and is hence a method to promote fuel quality. On the other hand, CO2 accumulation in the atmosphere causes global warming and requires effective route for its valorization. Utilization of CO2 as a carbon source for benzene alkylation could achieve both goals. Herein, alkylation of benzene with CO2 and H2 was realized by a series of low-cost bifunctional catalysts containing zinc/titanium oxides (Zn/Ti oxides) and HZSM-5 molecular sieves in a fixed-bed reactor. By regulating and controlling oxygen vacancies of Zn/Ti oxides and the acidities of HZSM-5, benzene conversion and CO2 conversion reached 28.7% and 29.9% respectively, along with a total selectivity of toluene and xylene higher than 90%. In this process, more than 25% CO2 was effectively utilized and incorporated into the target products. Moreover, the mechanism of the reaction was analyzed and the course was simultaneously traced. CO2 was transformed into methanol firstly, and then methanol reacted with benzene generating toluene and xylene. The innovation provides a new method for upgrading of fuels and upcycling the emissions of CO2, which is of great environmental and economic benefits.
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