Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles
Abstract
Renewable production of ammonia, a building block for most fertilizers, via the electrochemical nitrogen reduction reaction (ENRR) is desirable; however, a selective electrocatalyst is lacking. Here we show that vanadium nitride (VN) nanoparticles are active, selective, and stable ENRR catalysts with an ENRR rate and a Faradaic efficiency (FE) of 3.3 × 10–10 mol s–1 cm–2 and 6.0% at -0.1 V within 1 h, respectively. ENRR with 15N2 as the feed produces both 14NH3 and 15NH3, which indicates that the reaction follows a Mars–van Krevelen mechanism. Ex situ X-ray photoelectron spectroscopy characterization of fresh and spent catalysts reveals that multiple vanadium oxide, oxynitride, and nitride species are present on the surface and identified VN0.7O0.45 as the active phase in the ENRR. Operando X-ray absorption spectroscopy and catalyst durability test results corroborate this hypothesis and indicate that the conversion of VN0.7O0.45 to the VN phase leads to catalyst deactivation. We hypothesize that only the surface N sites adjacent to a surface O are active in the ENRR. Finally, an ammonia production rate of 1.1 × 10–10 mol s–1 cm–2 can be maintained for 116 h, with a steady-state turnover number of 431.
- Authors:
-
[1];
[1];
[1]
- Univ. of Delaware, Newark, DE (United States). Center for Catalytic Science and Technology, Dept. of Chemical and Biomolecular Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1484883
- Report Number(s):
- BNL-209653-2018-JAAM
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 41; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Yang, Xuan, Nash, Jared, Anibal, Jacob, Dunwell, Marco, Kattel, Shyam, Stavitski, Eli, Attenkofer, Klaus, Chen, Jingguang G., Yan, Yushan, and Xu, Bingjun. Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles. United States: N. p., 2018.
Web. doi:10.1021/jacs.8b08379.
Yang, Xuan, Nash, Jared, Anibal, Jacob, Dunwell, Marco, Kattel, Shyam, Stavitski, Eli, Attenkofer, Klaus, Chen, Jingguang G., Yan, Yushan, & Xu, Bingjun. Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles. United States. https://doi.org/10.1021/jacs.8b08379
Yang, Xuan, Nash, Jared, Anibal, Jacob, Dunwell, Marco, Kattel, Shyam, Stavitski, Eli, Attenkofer, Klaus, Chen, Jingguang G., Yan, Yushan, and Xu, Bingjun. Sun .
"Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles". United States. https://doi.org/10.1021/jacs.8b08379. https://www.osti.gov/servlets/purl/1484883.
@article{osti_1484883,
title = {Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles},
author = {Yang, Xuan and Nash, Jared and Anibal, Jacob and Dunwell, Marco and Kattel, Shyam and Stavitski, Eli and Attenkofer, Klaus and Chen, Jingguang G. and Yan, Yushan and Xu, Bingjun},
abstractNote = {Renewable production of ammonia, a building block for most fertilizers, via the electrochemical nitrogen reduction reaction (ENRR) is desirable; however, a selective electrocatalyst is lacking. Here we show that vanadium nitride (VN) nanoparticles are active, selective, and stable ENRR catalysts with an ENRR rate and a Faradaic efficiency (FE) of 3.3 × 10–10 mol s–1 cm–2 and 6.0% at -0.1 V within 1 h, respectively. ENRR with 15N2 as the feed produces both 14NH3 and 15NH3, which indicates that the reaction follows a Mars–van Krevelen mechanism. Ex situ X-ray photoelectron spectroscopy characterization of fresh and spent catalysts reveals that multiple vanadium oxide, oxynitride, and nitride species are present on the surface and identified VN0.7O0.45 as the active phase in the ENRR. Operando X-ray absorption spectroscopy and catalyst durability test results corroborate this hypothesis and indicate that the conversion of VN0.7O0.45 to the VN phase leads to catalyst deactivation. We hypothesize that only the surface N sites adjacent to a surface O are active in the ENRR. Finally, an ammonia production rate of 1.1 × 10–10 mol s–1 cm–2 can be maintained for 116 h, with a steady-state turnover number of 431.},
doi = {10.1021/jacs.8b08379},
journal = {Journal of the American Chemical Society},
number = 41,
volume = 140,
place = {United States},
year = {Sun Sep 23 00:00:00 EDT 2018},
month = {Sun Sep 23 00:00:00 EDT 2018}
}
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Figures / Tables:
Figure S1-1: Nitrogen adsorption isotherm for VN nanoparticles. The Brunauer−Emmett−Teller (BET) surface area is 177 m2 g−1.
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journal, January 2020
- Kugler, Kurt; Kriescher, Stefanie M. A.; Giela, Martin
- Chemie Ingenieur Technik, Vol. 92, Issue 1-2
Ammonia Synthesis Under Ambient Conditions: Selective Electroreduction of Dinitrogen to Ammonia on Black Phosphorus Nanosheets
journal, January 2019
- Zhang, Lili; Ding, Liang‐Xin; Chen, Gao‐Feng
- Angewandte Chemie, Vol. 131, Issue 9
A Combined Theory‐Experiment Analysis of the Surface Species in Lithium‐Mediated NH 3 Electrosynthesis
journal, April 2020
- Schwalbe, Jay A.; Statt, Michael J.; Chosy, Cullen
- ChemElectroChem, Vol. 7, Issue 7
Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction
journal, January 2020
- Huang, Yiyin; Babu, Dickson D.; Peng, Zhen
- Advanced Science, Vol. 7, Issue 4
Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions
journal, October 2019
- Wang, Xuesi; Xu, Chaochen; Jaroniec, Mietek
- Nature Communications, Vol. 10, Issue 1
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