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Reaction kinetics and temperature effects in syngas photo-initiated chemical vapor deposition on single-walled carbon nanotubes

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Abstract

Photo-initiated chemical vapor deposition (PICVD) is a solvent-free process that can be used to produce thin films on a variety of substrates, with applications in fields ranging from biomedicine to optics and microelectronics. This study presents a kinetic analysis for this process using syngas (CO + H2) as a precursor for the surface treatment of single-walled carbon nanotubes (SWCNT) with average dimensions of 1.5 × 100 nm (diameter × length), and addresses the role of iron pentacarbonyl (Fe(CO)5), a photo-active contaminant found in CO. This work builds upon previously developed reaction schemes for PICVD, based mainly on surface characterizations, by coupling these analyses with gas-phase monitoring. This allows us to propose two separate reaction schemes for the gas and surface phase reactions and consider temperature effects. Online FTIR, offline GC-MS, and online GC characterized the gas phase, while for surface characterizations, XPS and TGA were used. Characterizations showed that a coating with a general formula of CnO3nFen was deposited, corresponding to 0.29 ± 0.04 mg carbon and 0.49 ± 0.03 mg iron on the SWCNT substrate over the course of treatment. The Fe(CO)5 was identified as the key reactant in syngas/PICVD reactions and was nearly completely consumed (94%). Mass balances derived from the gas phase characterization showed that Fe(CO)5 inputted to the plug flow reactor could potentially contribute all the amount of 0.49 ± 0.03 mg of Fe and 0.29 ± 0.04 mg of C to the coating on the SWCNT, indicating that syngas/PICVD can be optimized in the future to decrease gas throughput. Temperature did not show a significant effect in the case of PICVD. However, in the absence of ultraviolet light, its role becomes determinant, with rising temperatures causing more Fe deposition.

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Acknowledgments

We wish to acknowledge the moral support from Polytechnique Montreal and Université de Sherbrooke. We would also like also to thank the Université de Sherbrooke Materials Characterization Laboratory, the Polytechnique Thin Films Group (GCM) and the microscopic characterization laboratory (CM)2. Also, special thanks to Mohammad Jaber Darabi and Gregory S. Patience for their assistance in GC-MS characterizations. The authors are also grateful to Ms. Josianne Lefebvre for her support in XPS analysis.

Funding

We wish to acknowledge the financial support provided by Fonds de recherche du Québec - Nature et technologies (FRQNT, grant no. 173942),

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Correspondence to Jason R. Tavares.

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Hosseininasab, S., Faucheux, N., Soucy, G. et al. Reaction kinetics and temperature effects in syngas photo-initiated chemical vapor deposition on single-walled carbon nanotubes. J Nanopart Res 21, 114 (2019). https://doi.org/10.1007/s11051-019-4558-6

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  • DOI: https://doi.org/10.1007/s11051-019-4558-6

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