期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 286, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.119929
关键词
Carbon dioxide hydrogenation; Aromatics synthesis; Bifunctional catalysis; HZSM-5 zeolites; ZnZrOx oxides
资金
- National Natural Science Foundation of China [21773286, U1832162, 91845105]
- Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21090204]
- Youth Innovation Promotion Association CAS [2018330]
- Shanghai Rising-Star Program, China [19QA1409900]
- Ministry of Science and Technology of China [2018YFB0604700, 2016YFA0202802]
- Chinese Academy of Sciences [ZDRW-ZS2018-1-3]
In this study, a series of bifunctional catalysts composed of highly active ZnZrOx oxides and nanocrystal HZSM-5 zeolites were used to achieve direct CO2 hydrogenation into aromatics with high selectivity. The extension of the b-axis length of HZSM-5 was found to increase the selectivity of para-xylene (PX) while shortening the length favored the formation of tetramethylbenzene (TeMB), with maximum selectivities reaching 28.9% and 74.1%, respectively.
Direct CO2 hydrogenation to high-value chemicals and fuels have received considerable attention. Nevertheless, efficiently producing aromatics with controllable aromatics distribution remains a great challenge. Herein, we report a series of bifunctional catalysts composed of highly active ZnZrOx oxides and nanocrystal HZSM-5 zeolites with the b-axis length ranging from 0.06 to 1.41 mu m, which enable direct CO2 hydrogenation into aromatics with high selectivity of 55-75 %. The CO2 conversion is up to 17.5 % with CO selectivity as low as 23.8 % mainly due to the affluent Brunsted acid sites and a large number of mesopores in HZSM-5 nanocrystal clusters with chain-like morphology. We demonstrate that a proper extension of the b-axis length of HZSM-5 can increase the selectivity of para-xylene (PX) while shortening the length of b-axis favors the formation of tetrame-thylbenzene (TeMB). The maximum selectivities of PX and TeMB in aromatics can reach to 28.9 % and 74.1 %, respectively.
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