Direct HCN synthesis via plasma-assisted conversion of methane and nitrogen

Kamarinopoulou, Nefeli S.; Wittreich, Gerhard R.; Vlachos, Dionisios G.

doi:10.1126/sciadv.adl4246

Title: Direct HCN synthesis via plasma-assisted conversion of methane and nitrogen

Journal Article · 29 March 2024 · Science Advances

DOI: https://doi.org/10.1126/sciadv.adl4246 · OSTI ID:2471801

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Univ. of Delaware, Newark, DE (United States); Univ. of Delaware, Newark, DE (United States)
Univ. of Delaware, Newark, DE (United States)

Hydrogen cyanide (HCN) is synthesized from ammonia (NH₃) and methane (CH₄) at ~1200°C over a Pt catalyst. Ammonia synthesis entails several complex, highly emitting processes. Plasma-assisted HCN synthesis directly from CH₄ and nitrogen (N₂) could be pivotal for on-demand HCN production. Here, we evaluate the potential of dielectric barrier discharge (DBD) N₂/CH₄ plasma for decentralized catalyst-free selective HCN production. We demonstrate a single-step conversion of methane and nitrogen to HCN with a 72% yield at <300°C. HCN is favored at low CH₄ concentrations with ethane (C₂H₆) as the secondary product. We propose a first-principles microkinetic model with few electron impact reactions. The model accurately predicts primary product yields and elucidates that methyl radical (·CH₃) is a common intermediate in HCN and C₂H₆ synthesis. Compared to current industrial processes, N₂/CH₄ DBD plasma can achieve minimal CO₂ emissions.

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Research Organization:: American Institute of Chemical Engineers (AIChE), New York, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0007888

OSTI ID:: 2471801

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 13 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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