Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 11, Issue 13, Pages 4521-4528Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cy00602a
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Funding
- Ministry of Science and Technology of China [2016YFA0202803, 2018YFA0704503]
- National Natural Science Foundation of China [91945302, 22008234, 22002153]
- Chinese Academy of Sciences [XDA21020400]
- Dalian High Level Talent Innovation Support Program [2017RD09]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2019184]
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The study reported an oxide-zeolite composite catalyst that enables the selective synthesis of para-xylene and light olefins from CO2 with renewable H-2, leading to higher yields of these valuable compounds. By modifying the zeolite with silica and phosphorus, the product selectivities can be significantly enhanced, providing a potential route for the synthesis of value-added chemicals using centralized greenhouse gas.
Catalytic hydrogenation of CO2 with renewable H-2 into valuable chemicals such as para-xylene and light olefins (C-2(=)-C-4(=)), which are important raw materials for the production of various commodities, is highly attractive. Herein we report that an oxide-zeolite (OXZEO) composite catalyst composed of ZnCrOx-ZSM-5 enables the selective synthesis of para-xylene and light olefins from CO2/H-2 in the presence of toluene. The product selectivities depend strongly on the acidity and location of acid sites of the zeolite function. By modifying ZSM-5 with silica, the external acid sites are shielded, and the pore openings are narrowed, which enhances significantly the formation of para-xylene. By modifying the zeolite with phosphorus, light olefins are co-produced due to the weakened acidity. As a result, the para-xylene fraction in xylene isomers reaches 82.8%, and the light olefin fraction in aliphatic hydrocarbons is as high as 75.8% when CO2 conversion is 20.9% and toluene conversion is 10.6%. Furthermore, the catalyst exhibits a good stability within a 100 h test. This provides a potential route for utilization of centralized greenhouse gas for synthesis of value-added chemicals.
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