Synergistically activating N2 and CO2 at water microdroplet interfaces

Zaifa Shi, Zuo-Chang Chen, Thomas Ka-Yam Lam, Jing Nie, Jianing Wang, Lei Guo, Yunkai Li, Haotian Ying, Xu Cai, Qingjie Zeng, Yanyan Chen, Lan-Sun Zheng, Zongwei Cai*

*Corresponding author for this work

Research output: Working paperPreprint

Abstract

Nitrogen (N2), one of the most stable molecules, can be fixed naturally by lightning. However, industrial nitrogen fixation via the Haber–Bosch and Ostwald processes is energy-intensive and exacerbates carbon dioxide (CO2) emissions. Meanwhile, CO2 has reached alarming atmospheric concentrations, rendering its efficient utilization a critical scientific challenge. Herein, we demonstrate that microdroplets generated by a sonic-spray array reactor can generate surface charges without an external electric field, enabling simultaneous activation of N2 and CO2 at the gas-water interfaces to form ammonium (NH4+, 84.3 µM), nitrate (NO3-, 5.7 µM) and formate (HCO2-, 16.5 µM) within 45 minutes. The activation processes of N2 and CO2 exhibits a synergistic enhancement effect at microdroplet interfaces. Mechanistic investigation reveals novel pathways involving the CO2-facilitated N2 activation and the oxygen radical (•O)-mediated N2 activation. Overall, this research offers a sustainable and energy-efficient strategy for green nitrogen fixation and utilizing CO2 from the atmosphere.
Original languageEnglish
PublisherChemRxiv
Number of pages23
DOIs
Publication statusPublished - 10 Jun 2025

User-Defined Keywords

  • Microdroplet
  • nitrogen fixation
  • Carbon dioxide activation
  • formate
  • nitrate
  • ammonium

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