Unraveling Nonequilibrium Generation of Atomic Nitrogen and Hydrogen in Plasma-Aided Ammonia Synthesis

Ning Liu, Xingqian Mao, Christopher Kondratowicz, Timothy Y. Chen, Bowen Mei, Ziyu Wang, Yijie Xu, Hongtao Zhong, Zhiyu Shi, Anatoli Morozov, Arthur Dogariu, Yiguang Ju

Research output: Contribution to journalArticlepeer-review

Abstract

Nonequilibrium generation of atomic nitrogen and hydrogen governing ammonia production both in the gas phase and on the catalyst surface is critical to plasma-aided ammonia synthesis. Here, this work studies the nonequilibrium generation of atomic nitrogen and hydrogen with a focus on the kinetic role of vibrational energy transfer of hydrogen molecules in plasma-aided ammonia synthesis. By combining two-photon absorption laser-induced fluorescence measurements and plasma kinetic modeling, we found that plasma not only generates ammonia but also produces critical H, N, and NH radicals via both electron impact and vibrational energy transfer excitations. The vibrational energy transfer from the excited hydrogen H2(v = 1) to higher vibrational levels H2(v = 2-3) via the V-V exchange (H2(v)-H2(v)) and V-V′ exchange (N2(v)-H2(v)) significantly enhances the H and NH production and then promotes the coupling between N and NH for ammonia synthesis both in the gas phase and on the catalyst surface.

Original languageEnglish (US)
Pages (from-to)2031-2036
Number of pages6
JournalACS Energy Letters
Volume9
Issue number5
DOIs
StatePublished - May 10 2024

All Science Journal Classification (ASJC) codes

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

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