Understanding the Activity and Stability of Vanadium Oxynitride Thin Films for N2 Reduction Reaction by Operando Measurements

Jinchao Wang^a, Johan-Michael Kurak^a, Anna B. Gunnarsdóttir^a, Tatiana Priamushko^e, Kevin Stojanovski^e, Arnar Sveinbjörnsson^b, Tryggvi K. Tryggvason^c, Erik Lewin^d, Fridrik Magnus^c^,^f, Árni S. Ingason^c, Árni B. Höskuldsson^a, Serhiy Cherevko^e, Egill Skúlason^a^,^b, Helga D. Flosadóttir^b

^aFaculty of Industrial Engineering, Mechanical Engineering and Computer Science, University of Iceland, VR-III, Reykjavík, Iceland

^bAtmonia ehf., Keldnaholt, 112 Reykjavík, Iceland.

^cGrein Research ehf., Dunhagi 5, 107 Reykjavík, Iceland.

^dInorganic Research Programme, Department of Chemistry – Ångström Laboratory, Uppsala University, 751 21 Uppsala, Sweden.

^eHelmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IET-2), Forschungszentrum Jülich, Cauerstr. 1, 91058 Erlangen, Germany.

^fScience Institute, University of Iceland, Dunhagi 5, 107 Reykjavik, Iceland

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)

Interlinking heterogeneous catalysts, mechanisms, and reactor concepts for dinitrogen reduction - #Nitroconversion

Sevilla, Spain, 2025 March 3rd - 7th

Organizers: Roland Marschall, Jennifer Strunk and Dirk Ziegenbalg

Poster, Jinchao Wang, 640
Publication date: 16th December 2024

The electrochemical nitrogen reduction reaction (eNRR) is an attractive approach with a promise of sustainable and low-carbon footprint alternative for ammonia synthesis. The current ammonia production process, i.e. Haber–Bosch, requires harsh conditions, high energy consumption, and is responsible for high CO₂ emission¹. The wide range of reported experimental results of eNRR has fascinated, yet troubled experimental and theoretical scientists in the past few years. False-positive results and poor replicability have plagued this study, partially due to natural concentrations of N-containing compounds in the environment and the catalysts ².

Significant theoretical and experimental work has focused on transition metal nitrides (TMN) as potential catalysts for the electrochemical N₂ fixation via the Mars-van Krevelen (MvK) mechanism^3–5. Although theoretical calculations indicate that metal nitrides are promising for NRR, experimental results have indicated spontaneous protonation of surface nitride ions to form NH₃. A computational work by Pan et al., suggested that the vanadium oxynitrides (VON) are promising catalysts for the NRR, where the presence of oxygen may play an important role in increasing the stability of V ions⁶. We will present a comprehensive electrochemical study paired with an operando NH₃ quantification system to investigate the activity and stability of VON, and for the first time introduce the S-number to NRR research which may hopefully benefit the further development of effective and rigorous evaluation of NRR catalysts.

References:

[1] MacFarlane, D. R. et al., Joule 4, 1186–1205 (2020). 2. Andersen, S. Z. et al., Nature 570, 504–508 (2019). 3. Abghoui, Y. et al., ACS Catal. 6, 635–646 (2016). 4. Yang, X. et al., J. Am. Chem. Soc. 140, 13387–13391 (2018). 5. Qiao, Z. et al., Cell Reports Physical Science 2, 100438 (2021). 6. Pan, J. et al., J. Mater. Chem. A 8, 24098–24107 (2020).

[2] Andersen, S. Z. et al., Nature 570, 504–508 (2019).

[3] Abghoui, Y. et al., ACS Catal. 6, 635–646 (2016).

[4] Yang, X. et al., J. Am. Chem. Soc. 140, 13387–13391 (2018)

[5] Qiao, Z. et al., Cell Reports Physical Science 2, 100438 (2021).

[6] Pan, J. et al., J. Mater. Chem. A 8, 24098–24107 (2020).

Acknowledgements:

This work was supported by the Icelandic Research Fund [grant numbers: 229082-051, 217896-051, and 196437-051], and the European Union, through project VERGE [HEU, GA: 101084253] and FIREFLY [HEU, GA: 101091715]. The views and opinions expressed are, however, those of the author(s) only and do not necessarily reflect those of the European Health and Digital Executive Agency (HADEA). Neither the European Union nor the granting authority can be held responsible for them.

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