Experimental and Computational Investigation of Hydrogen Evolution Reaction Mechanism on Nitrogen Functionalized Carbon Nanotubes

Sami Tuomi, Olli J. Pakkanen, Maryam Borghei, Rasmus Kronberg, Jani Sainio, Esko I. Kauppinen, Albert G. Nasibulin, Kari Laasonen, Tanja Kallio*

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

8 Citations (Scopus)
160 Downloads (Pure)

Abstract

Designing earth-abundant element based efficient and durable electrocatalysts for hydrogen evolution reaction (HER) is attracting growing attention as the renewable electricity supply sector urgently needs sustainable methods for storing energy. Nitrogen functionalized carbon nanomaterials are an interesting electrocatalysts option because of their attractive electrical properties, excellent chemical stability and catalytic activity. Hence, this study reports the HER mechanism on nitrogen functionalized few-walled carbon nanotubes (N-FWCNT). With this earth-abundant element based catalyst 250mV overpotential is required to reach 10mAcm-2 current density and so its HER activity is comparable to other non-noble metal catalysts, and clearly among the highest previously reported for N-FWCNTs. To gain fundament insight on their functioning, computational analysis has been carried out to verify the effect of nitrogen and to analyze the reaction mechanism. The reaction mechanism has also been analyzed experimentally with a pH series, and both the methods suggest that the HER proceeds via the Volmer-Heyrovský mechanism. Overall hydrogen surface coverage on N-FWCNT is also suggested to affect the HER rate. Interestingly, in the studied structure, carbons in vicinity of nitrogen atoms, but not directly bound to nitrogen, appear to promote the HER most actively. Furthermore, durability of N-FWCNTs has been demonstrated by operating a full electrolyzer cell for five weeks.

Original languageEnglish
Pages (from-to)3872-3882
JournalChemCatChem
Volume10
Issue number17
Early online date1 Jan 2018
DOIs
Publication statusPublished - 7 Sep 2018
MoE publication typeA1 Journal article-refereed

Keywords

  • Carbon nanotubes
  • Hydrogen evolution catalysis
  • Hydrogen reduction mechanism
  • Nitrogen doping

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    Critical raw material free electrocatalysis for hydrogen electrolyser

    Kallio, T., Rajala, T., Kauranen, P., Tuomi, S. & Muthuswamy, N.

    01/10/201615/10/2018

    Project: Academy of Finland: Other research funding

    Closing the Loop for High-added-value Materials

    Lahtinen, K., Kallio, T. & Revitzer, H.

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    Project: Academy of Finland: Strategic research funding

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