Molybdenum dioxide in carbon nanoreactors as a catalytic nanosponge for the efficient desulfurization of liquid fuels

Astle, Maxwell A.; Rance, Graham A.; Loughlin, Hannah J.; Peters, Thomas D.; Khlobystov, Andrei N.

Abstract

The principle of a “catalytic nanosponge” that combines the catalysis of organosulfur oxidation and sequestration of the products from reaction mixtures is demonstrated. Group VI metal oxide nanoparticles (CrOx, MoOx, WOx) are embedded within hollow graphitized carbon nanofibers (GNFs), which act as nanoscale reaction vessels for oxidation reactions used in the decontamination of fuel. When immersed in a model liquid alkane fuel contaminated with organosulfur compounds (benzothiophene, dibenzothiophene, dimethyldibenzothiophene), it is found that MoO2@GNF nanoreactors, comprising 30 nm molybdenum dioxide nanoparticles grown within the channel of GNFs, show superior abilities toward oxidative desulfurization (ODS), affording over 98% sulfur removal at only 5.9 mol% catalyst loading. The role of the carbon nanoreactor in MoO2@GNF is to enhance the activity and stability of catalytic centers over at least 5 cycles. Surprisingly, the nanotube cavity can selectively absorb and remove the ODS products (sulfoxides and sulfones) from several model fuel systems. This effect is related to an adsorptive desulfurization (ADS) mechanism, which in combination with ODS within the same material, yields a “catalytic nanosponge” MoO2@GNF. This innovative ODS and ADS synergistic functionality negates the need for a solvent extraction step in fuel desulfurization and produces ultralow sulfur fuel.

Citation

Astle, M. A., Rance, G. A., Loughlin, H. J., Peters, T. D., & Khlobystov, A. N. (2019). Molybdenum dioxide in carbon nanoreactors as a catalytic nanosponge for the efficient desulfurization of liquid fuels. Advanced Functional Materials, 29(17), Article 1808092. https://doi.org/10.1002/adfm.201808092

• Journal Article Type: Article
• Acceptance Date: Feb 27, 2019
• Online Publication Date: Feb 27, 2019
• Publication Date: Apr 25, 2019
• Deposit Date: Mar 21, 2019
• Publicly Available Date: Feb 28, 2020
• Journal: Advanced Functional Materials
• Print ISSN: 1616-301X
• Electronic ISSN: 1616-3028
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• Volume: 29
• Issue: 17
• Article Number: 1808092
• DOI: https://doi.org/10.1002/adfm.201808092
• Keywords: Electrochemistry; Electronic, Optical and magnetic materials; Condensed matter physics; Biomaterials
• Public URL: https://nottingham-repository.worktribe.com/output/1672541
• Publisher URL: https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.201808092
• Additional Information: This is the peer reviewed version of the following article: Astle, M. A., Rance, G. A., Loughlin, H. J., Peters, T. D., Khlobystov, A. N., Adv. Funct. Mater. 2019, 1808092. https://doi.org/10.1002/adfm.201808092 , which has been published in final form at https://doi.org/10.1002/adfm.201808092 . This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.