Rapid N<sub>2</sub>O Formation from N<sub>2</sub> on Water Droplet Surfaces

Abstract Nitrogen (N 2 ) has long been considered as stable atmospheric reservoir for N element and has a persistence time of hundreds of years. This study reveals that oxygen (O 2 ) at typical tropospheric concentrations can rapidly activate N 2 , leading to substantial production of nitrous oxide (N 2 O), the third most impactful greenhouse gas, at rates approaching 2.83±0.41 ppmv hour −1 catalyzed by ubiquitous water droplets in experimental systems. Notably, ozone (O 3 ), typically consumed by N 2 O in the stratosphere, can further accelerate N 2 O formation. In contrast, the produced N 2 O concentration is below detection limits in the absence of O 2 /O 3 or water droplets. A novel reduction‐then‐oxidation (RTO) mechanism was proposed to account for the rapid formation of N 2 O on the water droplet surfaces facilitated by the cooperation of water droplets and O 2 /O 3 . Further extrapolation indicates that the RTO pathway contributes several Tg N N 2 O annually, far exceeding the most known sources of N 2 O. These findings have broad implications for tracing atmospheric N 2 O sources, enhancing understanding of climate‐O 2 /O 3 interactions, and paving avenues for developing new methodologies for N 2 O synthesis.

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Publication Details

Journal
Angewandte Chemie
Published
2024-12-23
DOI
https://doi.org/10.1002/ange.202421002
Primary Topic
Air Quality Monitoring and Forecasting
Type
article
Field-Weighted Citation Impact
0.00

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article

Rapid N2O Formation from N2 on Water Droplet Surfaces

Huaijun Xie, Hong‐Bin Xie, Hai Zhang, Joseph S. Francisco et al.
Angewandte Chemie
Air Quality Monitoring and Forecasting
article

Rapid N2O Formation from N2 on Water Droplet Surfaces

Huaijun Xie, Hong‐Bin Xie, Hai Zhang, Joseph S. Francisco, Deming Xia, Rujing Yin, Jingwen Chen, Xiaofan Li, Qi Jiang, Jie Jiang
article en

Abstract

Abstract Nitrogen (N 2 ) has long been considered as stable atmospheric reservoir for N element and has a persistence time of hundreds of years. This study reveals that oxygen (O 2 ) at typical tropospheric concentrations can rapidly activate N 2 , leading to substantial production of nitrous oxide (N 2 O), the third most impactful greenhouse gas, at rates approaching 2.83±0.41 ppmv hour −1 catalyzed by ubiquitous water droplets in experimental systems. Notably, ozone (O 3 ), typically consumed by N 2 O in the stratosphere, can further accelerate N 2 O formation. In contrast, the produced N 2 O concentration is below detection limits in the absence of O 2 /O 3 or water droplets. A novel reduction‐then‐oxidation (RTO) mechanism was proposed to account for the rapid formation of N 2 O on the water droplet surfaces facilitated by the cooperation of water droplets and O 2 /O 3 . Further extrapolation indicates that the RTO pathway contributes several Tg N N 2 O annually, far exceeding the most known sources of N 2 O. These findings have broad implications for tracing atmospheric N 2 O sources, enhancing understanding of climate‐O 2 /O 3 interactions, and paving avenues for developing new methodologies for N 2 O synthesis.

Angewandte ChemieVol. 137(9)
Harbin Institute of Technology (CN), Dalian University of Technology (CN), Weihai Science and Technology Bureau (CN), University of Pennsylvania (US)
National Natural Science Foundation of China, National Postdoctoral Program for Innovative Talents, Fundamental Research Funds for the Central Universities
Openalex Percentile: Top 79%
Air Quality Monitoring and Forecasting
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