Coupling of N2 and O2 in the Gas Phase to Synthesize Nitric Oxide at Room Temperature: A Zeldovich-Like Strategy

Yong Qi Ding; Zhi Ying Chen; Feng Xiang Zhang; Jia Bi Ma

doi:10.1021/acs.jpclett.3c01675

Coupling of N₂ and O₂ in the Gas Phase to Synthesize Nitric Oxide at Room Temperature: A Zeldovich-Like Strategy

Yong Qi Ding, Zhi Ying Chen, Feng Xiang Zhang, Jia Bi Ma^*

^*Corresponding author for this work

Beijing Institute of Technology

Research output: Contribution to journal › Article › peer-review

1 Citation (Scopus)

Abstract

Dinitrogen (N₂) activation and its chemical transformations are some of the most challenging topics in chemistry. Herein, we report that heteronuclear metal anions AuNbBO^- can mediate the direct coupling of N₂ and O₂ to generate NO molecules. N₂ first forms the nondissociative adsorption product AuNbBON₂^- on AuNbBO^-. In the following reactions with two O₂ molecules, two NO molecules are gradually released, with the formation of AuNbBO₂N^- and AuNbBO₃^-. In the reaction with the first O₂, the generated nitrene radical (N^••-) originating from the dissociated N₂, induces the activation of O₂. Subsequently, the second O₂ is anchored and forms a superoxide radical (O₂^•-); this radical attacks the other N atom to form an N-O bond, releasing the second NO. The N^••- and O₂^•- radicals play key roles in the reactions. The mechanism adopted in this direct oxidation of N₂ by O₂ to NO can be labeled as a Zeldovich-like mechanism.

Original language	English
Pages (from-to)	7597-7602
Number of pages	6
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	34
DOIs	https://doi.org/10.1021/acs.jpclett.3c01675
Publication status	Published - 31 Aug 2023

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title = "Coupling of N2 and O2 in the Gas Phase to Synthesize Nitric Oxide at Room Temperature: A Zeldovich-Like Strategy",

abstract = "Dinitrogen (N2) activation and its chemical transformations are some of the most challenging topics in chemistry. Herein, we report that heteronuclear metal anions AuNbBO- can mediate the direct coupling of N2 and O2 to generate NO molecules. N2 first forms the nondissociative adsorption product AuNbBON2- on AuNbBO-. In the following reactions with two O2 molecules, two NO molecules are gradually released, with the formation of AuNbBO2N- and AuNbBO3-. In the reaction with the first O2, the generated nitrene radical (N••-) originating from the dissociated N2, induces the activation of O2. Subsequently, the second O2 is anchored and forms a superoxide radical (O2•-); this radical attacks the other N atom to form an N-O bond, releasing the second NO. The N••- and O2•- radicals play key roles in the reactions. The mechanism adopted in this direct oxidation of N2 by O2 to NO can be labeled as a Zeldovich-like mechanism.",

author = "Ding, {Yong Qi} and Chen, {Zhi Ying} and Zhang, {Feng Xiang} and Ma, {Jia Bi}",

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doi = "10.1021/acs.jpclett.3c01675",

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T1 - Coupling of N2 and O2 in the Gas Phase to Synthesize Nitric Oxide at Room Temperature

T2 - A Zeldovich-Like Strategy

AU - Ding, Yong Qi

AU - Chen, Zhi Ying

AU - Zhang, Feng Xiang

AU - Ma, Jia Bi

PY - 2023/8/31

Y1 - 2023/8/31

N2 - Dinitrogen (N2) activation and its chemical transformations are some of the most challenging topics in chemistry. Herein, we report that heteronuclear metal anions AuNbBO- can mediate the direct coupling of N2 and O2 to generate NO molecules. N2 first forms the nondissociative adsorption product AuNbBON2- on AuNbBO-. In the following reactions with two O2 molecules, two NO molecules are gradually released, with the formation of AuNbBO2N- and AuNbBO3-. In the reaction with the first O2, the generated nitrene radical (N••-) originating from the dissociated N2, induces the activation of O2. Subsequently, the second O2 is anchored and forms a superoxide radical (O2•-); this radical attacks the other N atom to form an N-O bond, releasing the second NO. The N••- and O2•- radicals play key roles in the reactions. The mechanism adopted in this direct oxidation of N2 by O2 to NO can be labeled as a Zeldovich-like mechanism.

AB - Dinitrogen (N2) activation and its chemical transformations are some of the most challenging topics in chemistry. Herein, we report that heteronuclear metal anions AuNbBO- can mediate the direct coupling of N2 and O2 to generate NO molecules. N2 first forms the nondissociative adsorption product AuNbBON2- on AuNbBO-. In the following reactions with two O2 molecules, two NO molecules are gradually released, with the formation of AuNbBO2N- and AuNbBO3-. In the reaction with the first O2, the generated nitrene radical (N••-) originating from the dissociated N2, induces the activation of O2. Subsequently, the second O2 is anchored and forms a superoxide radical (O2•-); this radical attacks the other N atom to form an N-O bond, releasing the second NO. The N••- and O2•- radicals play key roles in the reactions. The mechanism adopted in this direct oxidation of N2 by O2 to NO can be labeled as a Zeldovich-like mechanism.

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ER -

Coupling of N₂ and O₂ in the Gas Phase to Synthesize Nitric Oxide at Room Temperature: A Zeldovich-Like Strategy

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