Limitations of Electrochemical Nitrogen Oxidation toward Nitrate

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Standard

Limitations of Electrochemical Nitrogen Oxidation toward Nitrate. / Wan, Hao; Bagger, Alexander; Rossmeisl, Jan.

I: Journal of Physical Chemistry Letters, Bind 13, Nr. 38, 21.09.2022, s. 8928−8934.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt

Harvard

Wan, H, Bagger, A & Rossmeisl, J 2022, 'Limitations of Electrochemical Nitrogen Oxidation toward Nitrate', Journal of Physical Chemistry Letters, bind 13, nr. 38, s. 8928−8934. https://doi.org/10.1021/acs.jpclett.2c02459

APA

Wan, H., Bagger, A., & Rossmeisl, J. (2022). Limitations of Electrochemical Nitrogen Oxidation toward Nitrate. Journal of Physical Chemistry Letters, 13(38), 8928−8934. https://doi.org/10.1021/acs.jpclett.2c02459

Vancouver

Wan H, Bagger A, Rossmeisl J. Limitations of Electrochemical Nitrogen Oxidation toward Nitrate. Journal of Physical Chemistry Letters. 2022 sep. 21;13(38):8928−8934. https://doi.org/10.1021/acs.jpclett.2c02459

Author

Wan, Hao ; Bagger, Alexander ; Rossmeisl, Jan. / Limitations of Electrochemical Nitrogen Oxidation toward Nitrate. I: Journal of Physical Chemistry Letters. 2022 ; Bind 13, Nr. 38. s. 8928−8934.

Bibtex

@article{cff28d3c1ad5425a862127628c0445c2,
title = "Limitations of Electrochemical Nitrogen Oxidation toward Nitrate",
abstract = "The electrocatalytic N2 oxidation reaction (NOR) using renewable electricity is a promising alternative to the industrial synthesis of nitrate from NH3 oxidation. However, breaking the triple bond in the nitrogen molecule is one of the most essential challenges in chemistry. In this work, we use density functional theory simulations to investigate the plausible reaction mechanisms of electrocatalytic NOR and its competition with oxygen evolution reaction (OER) at the atomic scale. We focus on the electrochemical conversion of inert N2 to active *NO during NOR. We propose formation of *N2O from *N2 and *O as the rate-determining step (RDS). Following the RDS, a microkinetic model is utilized to study the rate of NOR on metal oxides. Our results demonstrate that a lower activation energy is obtained when a catalyst binds *O weakly. We show that the reaction is extremely challenging but also that design strategies have been suggested to promote electrochemical NOR.",
keywords = "REDUCTION, AMMONIA",
author = "Hao Wan and Alexander Bagger and Jan Rossmeisl",
year = "2022",
month = sep,
day = "21",
doi = "10.1021/acs.jpclett.2c02459",
language = "English",
volume = "13",
pages = "8928−8934",
journal = "Journal of Physical Chemistry Letters",
issn = "1948-7185",
publisher = "American Chemical Society",
number = "38",

}

RIS

TY - JOUR

T1 - Limitations of Electrochemical Nitrogen Oxidation toward Nitrate

AU - Wan, Hao

AU - Bagger, Alexander

AU - Rossmeisl, Jan

PY - 2022/9/21

Y1 - 2022/9/21

N2 - The electrocatalytic N2 oxidation reaction (NOR) using renewable electricity is a promising alternative to the industrial synthesis of nitrate from NH3 oxidation. However, breaking the triple bond in the nitrogen molecule is one of the most essential challenges in chemistry. In this work, we use density functional theory simulations to investigate the plausible reaction mechanisms of electrocatalytic NOR and its competition with oxygen evolution reaction (OER) at the atomic scale. We focus on the electrochemical conversion of inert N2 to active *NO during NOR. We propose formation of *N2O from *N2 and *O as the rate-determining step (RDS). Following the RDS, a microkinetic model is utilized to study the rate of NOR on metal oxides. Our results demonstrate that a lower activation energy is obtained when a catalyst binds *O weakly. We show that the reaction is extremely challenging but also that design strategies have been suggested to promote electrochemical NOR.

AB - The electrocatalytic N2 oxidation reaction (NOR) using renewable electricity is a promising alternative to the industrial synthesis of nitrate from NH3 oxidation. However, breaking the triple bond in the nitrogen molecule is one of the most essential challenges in chemistry. In this work, we use density functional theory simulations to investigate the plausible reaction mechanisms of electrocatalytic NOR and its competition with oxygen evolution reaction (OER) at the atomic scale. We focus on the electrochemical conversion of inert N2 to active *NO during NOR. We propose formation of *N2O from *N2 and *O as the rate-determining step (RDS). Following the RDS, a microkinetic model is utilized to study the rate of NOR on metal oxides. Our results demonstrate that a lower activation energy is obtained when a catalyst binds *O weakly. We show that the reaction is extremely challenging but also that design strategies have been suggested to promote electrochemical NOR.

KW - REDUCTION

KW - AMMONIA

U2 - 10.1021/acs.jpclett.2c02459

DO - 10.1021/acs.jpclett.2c02459

M3 - Journal article

C2 - 36130288

VL - 13

SP - 8928−8934

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

SN - 1948-7185

IS - 38

ER -

ID: 321268026