Cr/SSZ-13催化二氧化碳氧化乙烷脱氢反应的研究

doi:10.19964/j.issn.1006-4990.2021-0557

Abstract

Abstract:

The conversion of light alkanes into olefins with the same carbon number through dehydrogenation reaction is an important approach for high-value utilization of alkanes and diversification of olefin raw materials.Oxidative dehydrogenation of alkanes to olefins has been a hot issue due to its advantages such as no limit of reaction equilibrium,less carbon deposition and low reaction temperature.CRX/SSZ-13 series catalysts with different Cr loading were prepared by impregnation method.The physical properties of the catalysts were characterized by nitrogen physical adsorption,ammonia-temperature programmed desorption（NH₃-TPD）,carbon dioxide-temperature programmed desorption（CO₂-TPD）,hydrogen-temperature programmed reduction（H₂-TPR）,ultraviolet-visible spectroscopy（UV-Vis） and high-angle circular dark-field scanning transmission electron microscope（HAADF-STEM） coupled energy spectrum analysis（EDX-Mapping）.The catalytic performance of the catalysts for oxidative dehydrogenation of ethane to ethylene was evaluated in a micro fixed bed reactor.Finally,the structure-activity relationship of Cr/SSZ-13 catalyst was established.It was found that Cr_1.5/SSZ-13-10 catalyst[n（SiO₂）/n（Al₂O₃）=10] contained rich Cr³⁺ species,and the coordination unsaturated Cr³⁺ was an excellent dehydrogenation active site,which was co-nducive to the dehydrogenation of ethane by carbon dioxide oxidation.Therefore,Cr_1.5/SSZ-13-10 catalyst showed excellent catalytic performance at 650 ℃,the carbon dioxide conversion and ethane conversion reached 26.41% and 53.2%,respectively,and the ethylene yield was 38.83%.

Key words: Cr/SSZ-13, carbon dioxide, oxidative dehydrogenation, ethane, ethylene

CLC Number:

O643.36

ZHOU Wei,YU Haibin,MA Xinbin. Oxidative dehydrogenation of ethane with carbon dioxide to ethylene over Cr/SSZ-13 catalyst[J]. Inorganic Chemicals Industry, 2021, 53(12): 43-48.

Figures/Tables 9

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样品	S_BET/（m²·g^-1）	S_micro/（m²·g^-1）	S_exter/（m²·g^-1）	V_pores/（cm³·g^-1）	V_micro/（cm³·g^-1）	V_meso/（cm³·g^-1）
SSZ-13-10	654	613	41	0.33	0.24	0.09
Cr_0.5/SSZ-13-10	642	601	40	0.33	0.24	0.09
Cr_1.0/SSZ-13-10	623	583	41	0.32	0.23	0.09
Cr_1.5/SSZ-13-10	601	560	41	0.30	0.22	0.08
Cr_2.5/SSZ-13-10	564	525	39	0.28	0.21	0.07
SSZ-13-50	762	734	28	0.36	0.30	0.06
Cr_1.0/SSZ-13-50	744	720	25	0.35	0.29	0.06
Cr_1.5/SSZ-13-50	685	658	27	0.33	0.27	0.06
Cr_2.0/SSZ-13-50	677	653	24	0.33	0.27	0.06

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Oxidative dehydrogenation of ethane with carbon dioxide to ethylene over Cr/SSZ-13 catalyst

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