Disproportionation of nitrogen induced by DC plasma-driven electrolysis in a nitrogen atmosphere

Pattyn, Cédric; Maira, Nicolas; Buddhadasa, Madhuwanthi; Vervloessem, Elise; Iséni, Sylvain; Roy, Narayan; Rémy, Antoine; Delplancke, Marie-Paule; Reniers, François

doi:10.1039/d2gc01013e

Cited by 9 publications

(10 citation statements)

References 77 publications

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“…Muzammil et al [ 106 ] conducted a study on NF using a RGA reactor with tangential air input, driven by a 20 kHz AC power supply. The research found that lower SEI resulted in lower energy consumption, which is consistent with the conclusions of Pei et al [ 104 ] and Pattyn et al [ 91 ] The lowest energy consumption for NF was found to be approximately 0.67 MJ/mol.…”

Section: Recent Progress On Plasma Nfsupporting

confidence: 89%

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Plasma for nitrogen fixation by using N₂/O₂ mixture: Reaction pathway, energy flow, and plasma reactor

Liu,

Nie,

Liu

et al. 2023

Plasma Processes & Polymers

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When N2/O2 mixture is used for nitrogen fixation (NF), researchers believe that the Zeldovich mechanism is the main pathway for NO formation. However, there is still debate on whether N2 participates in the Zeldovich mechanism through vibrational excitation or electronic excitation of the N2(A) state. This ambiguity has led to uncertainty regarding which type of plasma can achieve higher efficiency. Furthermore, the most significant obstacle to plasma‐assisted NF is the high energy consumption. Gaining a deeper understanding of the energy flow in the discharge process is crucial for improving NF energy efficiency in the future. Therefore, this paper provides an overview of the research on these topics. Finally, various new plasma NF devices reported in recent years will also be discussed.

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Section: Recent Progress On Plasma Nfsupporting

confidence: 89%

“…Pattyn et al [ 91 ] further investigated NF on the water surface using DC negative high voltage and studied the impact of adding water vapor to the nitrogen gas on the NF efficiency. They found that the best NF efficiency was achieved when adding 6–8 mol% water vapor, leading to lowest energy consumption of 61.6 MJ/mol.…”

Section: Recent Progress On Plasma Nfmentioning

confidence: 99%

Plasma for nitrogen fixation by using N₂/O₂ mixture: Reaction pathway, energy flow, and plasma reactor

Liu,

Nie,

Liu

et al. 2023

Plasma Processes & Polymers

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“…Up to date, several catalytic systems have been demonstrated to have a potential of activating the super-strong N≡N triplebond, however their practical applications are yet to be explored [15][16][17] . N2 fixation into NH3 and NOy (NO, NO2, NO3, HNO3, HNO2, etc) has been reported in several plasmabased methods 10,12,18 . However, NOy are toxic to the environment.…”

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confidence: 99%

Ambient catalyst free nitrogen fixation with water dimer radical cation

Zhang

Huang

et al. 2023

Preprint

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The growth and sustainable development of humanity is heavily dependent upon the process of fixing nitrogen (N2) to ammonia (NH3). However, the currently adopted methods are associated with severe environmental hazards and tremendous energy costs, which limit their sustainability and profitability. Herein we discovered a catalyst-free disproportionation reaction of N2 by water dimer radical cation, (H2O)2+•, which occurs under mild ambient conditions via distinctive HONH-HNOH+• intermediate to yield economically valuable nitroxyl (HNO) and hydroxylamine (NH2OH) products, in alternative to NH3. Calculations suggest that the reaction is prompted by the coordination of electronically excited N2 with (H2O)2+• in its two-center-three-electron (2c-3e) configuration. Subsequent excited-state double proton transfer leads to one-step water addition to N2. The ambient fixation of N2 into HNO and NH2OH with high selectivity offers great profitability and total avoidance of polluting emissions, such as CO2 or NOy, thus giving an entirely new look and perspectives to the problem of green N2 fixation.

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“…Up to date, several catalytic systems have been demonstrated to have a potential of activating the super-strong N≡N triple-bond, however their practical applications are yet to be explored (15)(16)(17). N2 fixation into NH3 and NOy (NO, NO2, NO3, HNO3, HNO2, etc) has been reported in several plasma-based methods (10,12,18). However, NOy are toxic to the environment.…”

mentioning

confidence: 99%

Ambient catalyst-free nitrogen fixation with water dimer

Zhang

Huang

et al. 2023

Preprint

View full text Add to dashboard Cite

The growth and sustainable development of humanity is heavily dependent upon the process of fixing nitrogen (N2) to ammonia (NH3). However, the currently adopted methods are associated with severe environmental hazards and tremendous energy costs, which limit their sustainability and profitability. Herein we discovered a catalyst-free disproportionation reaction of N2 by water dimer radical cation, (H2O)2+, which occurs under mild ambient conditions via distinctive HONH-HNOH+ intermediate to yield economically valuable nitroxyl (HNO) and hydroxylamine (NH2OH) products, in alternative to NH3. Calculations suggest that the reaction is prompted by the coordination of electronically excited N2 with (H2O)2+ in its two-center-three-electron (2c-3e) configuration. The ambient one-step fixation of N2 into HNO and NH2OH with high selectivity offers great profitability and total avoidance of polluting emissions, such as CO2 or NOy, thus giving an entirely new look and perspectives to the problem of green N2 fixation.

show abstract

Disproportionation of nitrogen induced by DC plasma-driven electrolysis in a nitrogen atmosphere

Abstract: Nitrogen disproportionation i.e. its simultaneous conversion to compounds of higher (NOx) and lower (NH3) oxidation states in a N2 DC plasma-driven electrolysis process with a plasma cathode is investigated. This...

Cited by 9 publications

References 77 publications

Plasma for nitrogen fixation by using N₂/O₂ mixture: Reaction pathway, energy flow, and plasma reactor

Plasma for nitrogen fixation by using N₂/O₂ mixture: Reaction pathway, energy flow, and plasma reactor

Ambient catalyst free nitrogen fixation with water dimer radical cation

Ambient catalyst-free nitrogen fixation with water dimer

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Disproportionation of nitrogen induced by DC plasma-driven electrolysis in a nitrogen atmosphere

Abstract: Nitrogen disproportionation i.e. its simultaneous conversion to compounds of higher (NOx) and lower (NH3) oxidation states in a N2 DC plasma-driven electrolysis process with a plasma cathode is investigated. This...

Cited by 9 publications

References 77 publications

Plasma for nitrogen fixation by using N2/O2 mixture: Reaction pathway, energy flow, and plasma reactor

Plasma for nitrogen fixation by using N2/O2 mixture: Reaction pathway, energy flow, and plasma reactor

Ambient catalyst free nitrogen fixation with water dimer radical cation

Ambient catalyst-free nitrogen fixation with water dimer

Contact Info

Product

Resources

About

Plasma for nitrogen fixation by using N₂/O₂ mixture: Reaction pathway, energy flow, and plasma reactor

Plasma for nitrogen fixation by using N₂/O₂ mixture: Reaction pathway, energy flow, and plasma reactor