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氧化铟负载氧化锆与硅铝磷酸分子筛 34 混合催化剂在二氧化碳加氢制低碳烯烃中的协同增效作用。

Effective synergies in indium oxide loaded with zirconia mixed with silicoaluminophosphate molecular sieve number 34 catalysts for carbon dioxide hydrogenation to lower olefins.

机构信息

School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, PR China.

School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, PR China.

出版信息

J Colloid Interface Sci. 2023 Apr;635:148-158. doi: 10.1016/j.jcis.2022.12.086. Epub 2022 Dec 20.

DOI:10.1016/j.jcis.2022.12.086
PMID:36584615
Abstract

Tandem catalysts consisting of metal oxides and zeolites have been widely studied for catalytic carbon dioxide (CO) hydrogenation to lower olefins, while the synergies of two components and their influence on the catalytic performance are still unclear. In this study, the composite catalysts composed of indium oxide loaded with zirconia (InO/ZrO) and silicoaluminophosphate molecular sieve number 34 (SAPO-34) are developed. Performance results indicate that the synergies between these two components can promote CO hydrogenation. Further characterizations reveal that the chabazite (CHA) structure and acid sites in the SAPO-34 are destroyed when preparing In-Zr/SAPO by powder milling (In-Zr/SAPO-M) because of the excessive proximity of two components, which inhibits the activation of CO and hydrogen (H), thus resulting in much higher methane selectivity than the catalysts prepared by granule stacking (In-Zr/SAPO-G). Proper granule integration manner promotes tandem reaction, thus enhancing CO hydrogenation to lower olefins, which can provide a practicable strategy to improve catalytic performance and the selectivity of the target products.

摘要

串联催化剂由金属氧化物和沸石组成,已广泛研究用于催化二氧化碳(CO)加氢转化为低碳烯烃,但两种组分的协同作用及其对催化性能的影响仍不清楚。在这项研究中,开发了由负载氧化铟的氧化锆(InO/ZrO)和硅铝磷酸分子筛 34(SAPO-34)组成的复合催化剂。性能结果表明,这两种组分之间的协同作用可以促进 CO 加氢。进一步的表征表明,当通过粉末研磨(In-Zr/SAPO-M)制备 In-Zr/SAPO 时,SAPO-34 中的 CHA 结构和酸位由于两种组分过于接近而被破坏,这抑制了 CO 和氢气(H)的活化,从而导致甲烷选择性比通过颗粒堆积(In-Zr/SAPO-G)制备的催化剂高得多。适当的颗粒集成方式促进了串联反应,从而提高了 CO 加氢转化为低碳烯烃的效率,这为提高催化性能和目标产物的选择性提供了一种可行的策略。

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