期刊
ACS CATALYSIS
卷 9, 期 2, 页码 895-901出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b01344
关键词
CO2 conversion; aromatics synthesis; bifunctional catalysts; tandem process; single pass
资金
- JST-ACT-C project of the Japan Science and Technology Agency, Japan [JPMJCR12YT]
- JST-MIRAI project of the Japan Science and Technology Agency, Japan [JPMJMI17E2]
- National Natural Science Foundation of China [91645113, U1510110]
- Key Research Program of Frontier Sciences, CAS [QYZDB-SSW-JSC043]
The efficient conversion of CO2 to useful chemicals is a promising way to reduce atmospheric CO2 concentration and also reduce reliance on fossil-based resources. Although much progress has been made toward the production of basic chemicals, like methanol, through CO2 hydrogenation, the direct conversion of CO2 to value-added aromatics, especially p-xylene (PX), is still a great challenge due to the inert nature of CO2 and high barrier for C-C coupling. Herein, a bifunctional catalyst composed of Cr2O3 and H-ZSM-5 zeolite (Cr2O3/H-ZSM-5) was designed for the direct conversion of CO2 to aromatics. Due to the concertedly synergistic effect between the two components in this bifunctional catalyst, aromatics selectivity of, similar to 76% at CO2 conversion of 34.5% was achieved, and there was no catalyst deactivation after 100 h of long-term stability testing. Moreover, a modified bifunctional catalyst Cr2O3/H-ZSM-5@S-1 (silicalite-1) consisting of a core-shell structured H-ZSM-5@S-1 zeolite capsule component was proposed to realize the target synthesis of BTX (benzene, toluene, and xylene), especially PX. The precise suppression of undesired side reactions was accomplished on Cr2O3/H-ZSM-5@S-1 because neutralizing acidic sites at outer surface of H-ZSM-5 by S-1 stopped isomerization of PX to o- or m-xylene as well as other side reactions. Consequently, the fractions of BTX and PX in aromatics products were increased from 13.2% and 7.6% to 43.6% and 25.3%, respectively, with almost unchanged catalyst activity and total aromatics selectivity.
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