Please use this identifier to cite or link to this item:
http://dx.doi.org/10.18419/opus-14973
Authors: | Glauber, Jean-Pierre Lorenz, Julian Liu, Ji Müller, Björn Bragulla, Sebastian Kostka, Aleksander Rogalla, Detlef Wark, Michael Nolan, Michael Harms, Corinna Devi, Anjana |
Title: | A sustainable CVD approach for ZrN as a potential catalyst for nitrogen reduction reaction |
Issue Date: | 2024 |
metadata.ubs.publikation.typ: | Zeitschriftenartikel |
metadata.ubs.publikation.seiten: | 15451-15464 |
metadata.ubs.publikation.source: | Dalton transactions 53 (2024), S. 15451-15464 |
URI: | http://nbn-resolving.de/urn:nbn:de:bsz:93-opus-ds-149929 http://elib.uni-stuttgart.de/handle/11682/14992 http://dx.doi.org/10.18419/opus-14973 |
ISSN: | 1477-9234 1477-9226 |
Abstract: | In pursuit of developing alternatives for the highly polluting Haber-Bosch process for ammonia synthesis, the electrocatalytic nitrogen reduction reaction (NRR) using transition metal nitrides such as zirconium mononitride (ZrN) has been identified as a potential pathway for ammonia synthesis. In particular, specific facets of ZrN have been theoretically described as potentially active and selective for NRR. Major obstacles that need to be addressed include the synthesis of tailored catalyst materials that can activate the inert dinitrogen bond while suppressing hydrogen evolution reaction (HER) and not degrading during electrocatalysis. To tackle these challenges, a comprehensive understanding of the influence of the catalyst's structure, composition, and morphology on the NRR activity is required. This motivates the use of metal–organic chemical vapor deposition (MOCVD) as the material synthesis route as it enables catalyst nanoengineering by tailoring the process parameters. Herein, we report the fabrication of oriented and facetted crystalline ZrN thin films employing a single source precursor (SSP) MOCVD approach on silicon and glassy carbon (GC) substrates. First principles density functional theory (DFT) simulations elucidated the preferred decomposition pathway of SSP, whereas ab initio molecular dynamics simulations show that ZrN at room temperature undergoes surface oxidation with ambient O2, yielding a Zr-O-N film, which is consistent with compositional analysis using Rutherford backscattering spectrometry (RBS) in combination with nuclear reaction analysis (NRA) and X-ray photoelectron spectroscopy (XPS) depth profiling. Proof-of-principle electrochemical experiments demonstrated the applicability of the developed ZrN films on GC for NRR and qualitatively hint towards a possible activity for the electrochemical NRR in the sulfuric acid electrolyte. A versatile CVD process for growing facetted ZrN layers as a potential catalyst for electrochemical reduction of nitrogen to ammonia. |
Appears in Collections: | 04 Fakultät Energie-, Verfahrens- und Biotechnik |
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