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Ga CrO /H-SAPO-34(F), a highly efficient bifunctional catalyst for the direct conversion of CO2 into ethene and propene

丙烯 双功能 催化作用 化学 材料科学 有机化学
作者
Wenyu Zhang,Sen Wang,Shujia Guo,Zhangfeng Qin,Mei Dong,Weibin Fan,Jianguo Wang
出处
期刊:Fuel [Elsevier BV]
卷期号:329: 125475-125475 被引量:20
标识
DOI:10.1016/j.fuel.2022.125475
摘要

Adding Ga in Ga m CrO x can regulate the adsorption and activation of CO 2 and H 2 , whereas adding HF during synthesis can modulate the acidity of H-SAPO-34 ( n F). The Ga 0.15 CrO x /H-SAPO-34(0.5/1.0 F) composite exhibits excellent performance in the direct hydrogenation of CO 2 to light olefins. • Ga m CrO x /H-SAPO-34(F) shows excellent catalytic performance in CO 2 to light olefins. • Ga 0.15 CrO x has pertinent oxygen vacancies and moderate CO 2 and H 2 adsorption strength. • Adding HF during synthesis can modulate the acid quantity and strength of H-SAPO-34. • Product spectrum of CO 2 hydrogenation can be regulated over Ga m CrO x /H-SAPO-34(F). • Olefins product is concentrated in ethene and in particular propene (C 2 = –C 3 = > 94 %). The conversion of CO 2 into light olefins is considered as an effective route for the sustainable production of valuable chemicals as well as the remission of global warning induced by excessive CO 2 emission; however, it is still rather challenging to get a catalyst with satisfactorily high yield for the target products. Herein, we designed a new bifunctional Ga m CrO x /H-SAPO-34( n F) catalyst, which exhibits excellent performance in the direct hydrogenation of CO 2 to light olefins; the selectivity to ethene, propene and butenes (C 2 = –C 4 = ) reaches 87.3 % (excluding CO) at a CO 2 conversion of 11.9 % and selectivity of 34.5 % to CO, at 350 °C and 3.0 MPa. Various characterization results indicate that the structure and performance of Ga m CrO x oxide moiety is related to the Ga/Cr molar ratio ( m ); Ga 0.15 CrO x is provided with abundant oxygen vacancies and moderate CO 2 and H 2 adsorption strength and can effectively catalyze the hydrogenation of CO 2 to methanol and related intermediates. In addition, adding proper amount of HF during the synthesis of H-SAPO-34( n F) zeotype moiety can modulate the quantity and strength of Brønsted acid sites and then meliorate the C C bond coupling and cracking reactions. As a result, for the CO 2 hydrogenation over the Ga 0.15 CrO x /H-SAPO-34(F) composite catalyst, ethene and propene predominate the light olefins product (accounting for above 94 %), whereas higher olefins are greatly suppressed. Current work supplies a practical measure or helpful hint for the design of efficient catalysts in the selective conversion of CO 2 to target olefins.
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