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定制源自MIL-100(Fe)的催化剂以实现可控的二氧化碳转化和产物选择性。

Tailoring MIL-100(Fe)-derived catalyst for controlled carbon dioxide conversion and product selectivity.

作者信息

Ahmed Hany E, Albolkany Mohamed K, El-Khouly Mohamed E, El-Moneim Ahmed Abd

机构信息

Nanoscience Program, Institute of Basic and Applied Sciences, Egypt-Japan University of Science and Technology New Borg El-Arab City Alexandria 21934 Egypt

National Institute of Standards Tersa St, El-Matbah, Haram, P. O. Box: 136, Code No 12211 Giza Egypt.

出版信息

RSC Adv. 2024 Apr 29;14(20):13946-13956. doi: 10.1039/d4ra01772b. eCollection 2024 Apr 25.

Abstract

Here in, we are reporting the effect of the catalyst particle size on the catalytic activity and product selectivity by understanding the strength of the interaction between the active catalyst and the reactants (CO and H). In this regard, two catalytic systems having different active catalyst particle sizes and support surface areas were synthesized using metal-organic frameworks (MOF) (MIL-100(Fe)) having two crystal size ranges as sacrificial templates. The active catalyst having smaller nanoparticles exhibited greater chemisorption of hydrogen (Fe-H bond), resulting in heightened selectivity for paraffin due to hydrogenation of re-adsorbed olefins. Conversely, larger nanoparticles showed enhanced chemisorption of CO (Fe-C bond), leading to increased selectivity for olefins (O/P = 0.15). Additionally, a reduction in particle size boosts activity from 24% to 38.7% at 340 °C/20 bar. While, higher particle size enhances the selectivity towards C from 11.1 to 45.6% at (300 °C/10 bar) and 9.6 to 21.3% at (340 °C/20 bar).

摘要

在此,我们通过了解活性催化剂与反应物(CO和H)之间相互作用的强度,来报告催化剂粒径对催化活性和产物选择性的影响。在这方面,使用具有两种晶体尺寸范围的金属有机框架(MOF)(MIL-100(Fe))作为牺牲模板,合成了具有不同活性催化剂粒径和载体表面积的两种催化体系。具有较小纳米颗粒的活性催化剂表现出对氢更强的化学吸附(Fe-H键),由于再吸附烯烃的氢化作用,导致对石蜡的选择性提高。相反,较大的纳米颗粒显示出对CO更强的化学吸附(Fe-C键),导致对烯烃的选择性增加(O/P = 0.15)。此外,在340°C/20巴的条件下,粒径减小会使活性从24%提高到38.7%。同时,在(300°C/10巴)时,较大粒径会使对C的选择性从11.1%提高到45.6%,在(340°C/20巴)时从9.6%提高到21.3%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ad70/11056685/d921ba0637da/d4ra01772b-f1.jpg

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