Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles

Yang, Xuan; Nash, Jared; Anibal, Jacob; Dunwell, Marco; Kattel, Shyam; Stavitski, Eli; Attenkofer, Klaus; Chen, Jingguang G.; Yan, Yushan; Xu, Bingjun

doi:10.1021/jacs.8b08379

Title: Mechanistic Insights into Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Nanoparticles

Journal Article · 22 September 2018 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.8b08379 · OSTI ID:1484883

^[1]; Nash, Jared ^[1]; Anibal, Jacob ^[1]; Dunwell, Marco ^[1]; Kattel, Shyam ^[2]; Stavitski, Eli ^[3]; Attenkofer, Klaus ^[3]; Chen, Jingguang G. ^[2];

^[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)

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 VN_0.7O0.45 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1484883

Report Number(s):: BNL--209653-2018-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 41 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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ZnO Quantum Dots Coupled with Graphene toward Electrocatalytic N ₂ Reduction: Experimental and DFT Investigations Liu, Ya‐ping; Li, Yu‐biao; Huang, Da‐jian Chemistry – A European Journal, Vol. 25, Issue 51 https://doi.org/10.1002/chem.201902156	journal	August 2019
B ₄ C nanosheets decorated with in situ -derived boron-doped graphene quantum dots for high-efficiency ambient N ₂ fixation Qiu, Wei-Bin; Luo, Yu-Xi; Liang, Ru-Ping Chemical Communications, Vol. 55, Issue 51 https://doi.org/10.1039/c9cc03413g	journal	January 2019
Boron and nitrogen co-doped porous carbon nanofibers as metal-free electrocatalysts for highly efficient ammonia electrosynthesis Kong, Yan; Li, Yan; Yang, Bin Journal of Materials Chemistry A, Vol. 7, Issue 46 https://doi.org/10.1039/c9ta06076f	journal	January 2019
Electrochemical nitrogen fixation and utilization: theories, advanced catalyst materials and system design Guo, Wenhan; Zhang, Kexin; Liang, Zibin Chemical Society Reviews, Vol. 48, Issue 24 https://doi.org/10.1039/c9cs00159j	journal	January 2019
High Efficiency Electrochemical Nitrogen Fixation Achieved with a Lower Pressure Reaction System by Changing the Chemical Equilibrium Cheng, Hui; Cui, Peixin; Wang, Fangrui Angewandte Chemie, Vol. 131, Issue 43 https://doi.org/10.1002/ange.201910658	journal	September 2019
Quantification of Active Sites and Elucidation of the Reaction Mechanism of the Electrochemical Nitrogen Reduction Reaction on Vanadium Nitride Yang, Xuan; Kattel, Shyam; Nash, Jared Angewandte Chemie, Vol. 131, Issue 39 https://doi.org/10.1002/ange.201906449	journal	August 2019
Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction Huang, Yiyin; Babu, Dickson D.; Peng, Zhen Advanced Science, Vol. 7, Issue 4 https://doi.org/10.1002/advs.201902390	journal	January 2020
Biomass-derived oxygen-doped hollow carbon microtubes for electrocatalytic N ₂ -to-NH ₃ fixation under ambient conditions Wu, Tengteng; Li, Peipei; Wang, Huanbo Chemical Communications, Vol. 55, Issue 18 https://doi.org/10.1039/c8cc09867k	journal	January 2019
The doping and oxidation of 2D black and blue phosphorene: a new photocatalyst for nitrogen reduction driven by visible light Cheng, Yuwen; Song, Yan; Zhang, Yumin Physical Chemistry Chemical Physics, Vol. 21, Issue 44 https://doi.org/10.1039/c9cp04647j	journal	January 2019

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