Plasma nitrogen fixation in the presence of a liquid interface: role of OH radicals

Gromov, Mikhail; Leonova, Kseniia; Britun, Nikolay; Degeyter, Nathalie; Morent, Rino; Snyders, Rony; Nikiforov, Anton

doi:10.1039/d2re00014h

Cited by 6 publications

(9 citation statements)

References 21 publications

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“…[31] Building upon existing research, future investigations may focus on inhibiting reactions between oxidative species (such as OH radicals and O atoms) and nitrogen species, as well as suppressing hydrogen evolution reactions, to further enhance ammonia synthesis selectivity. [93] Research into the generation of different reactive nitrogen species and their respective reactivity with oxidants and reductants could lead to breakthroughs. [94] This exploration can provide insights into adjusting reaction conditions to promote the formation of active nitrogen species favorable for ammonia synthesis.…”

Section: Reaction Selectivitymentioning

confidence: 99%

“…These radicals then react with reactive nitrogen species, resulting in the production of nitrogen oxides that dissolve in water and ultimately form nitrate and nitrite species through a series of reactions. While this type of reactions is acceptable for nitrogen fixation purposes, it presents a challenge for the plasma‐assisted ammonia synthesis as it competes with the desired reaction, utilizing reactive nitrogen species and generating byproducts that reduce the ammonia yield [93] . Therefore, improving the selectivity of the plasma nitrogen‐water system has become a key objective in the ammonia synthesis research.…”

Section: Plasma‐assisted Synthesis Of Nh3 From N2 and H2omentioning

confidence: 99%

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Plasma‐Assisted Sustainable Nitrogen‐to‐Ammonia Fixation: Mixed‐phase, Synergistic Processes and Mechanisms

Qu,

Zhou,

Sun

et al. 2023

ChemSusChem

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Ammonia plays a crucial role in industry and agriculture worldwide, but traditional industrial ammonia production methods are energy‐intensive and negatively impact the environment. Ammonia synthesis using low‐temperature plasma technology has gained traction in the pursuit of environment‐benign and cost‐effective methods for producing green ammonia. This Review discusses the recent advances in low‐temperature plasma‐assisted ammonia synthesis, focusing on three main routes: N2+H2 plasma‐only, N2+H2O plasma‐only, and plasma coupled with other technologies. The reaction pathways involved in the plasma‐assisted ammonia synthesis, as well as the process parameters, including the optimum catalyst types and discharge schemes, are examined. Building upon the current research status, the challenges and research opportunities in the plasma‐assisted ammonia synthesis processes are outlined. The article concludes with the outlook for the future development of the plasma‐assisted ammonia synthesis technology in real‐life industrial applications.

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Section: Reaction Selectivitymentioning

confidence: 99%

Section: Plasma‐assisted Synthesis Of Nh3 From N2 and H2omentioning

confidence: 99%

Plasma‐Assisted Sustainable Nitrogen‐to‐Ammonia Fixation: Mixed‐phase, Synergistic Processes and Mechanisms

Qu,

Zhou,

Sun

et al. 2023

ChemSusChem

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“…Currently, relevant studies have been carried out to reveal the chemical mechanism of NO x generation from NTPNF through experiments or simulations. Vibrational excitation of N 2 and O 2 molecules provides the energy required to overcome the activation barrier for the nonthermal Zeldovich mechanism. ,,,, It involves two crucial steps: the reaction of excited-state N 2 (v) molecules and O• radicals (R1) and the reaction of excited-state O 2 (v) molecules to N• radicals (R2) (where v represents vibrationally excited states). − Furthermore, the participation of water vapor can further extend the Zeldovich mechanism: the N• radical forms NO (R3) by reacting with the OH produced by hydrolysis. − For the catalytic mechanism, some studies have proposed the Eley–Rideal (E-R) and Langmuir–Hinshelwood (L-H) mechanisms with density functional theory (DFT) calculations, ,, but the reasons for choosing these two mechanisms or the modes for their actions were not investigated. Furthermore, these mechanism studies do not fully take into account the coupling with plasma, which is essential for developing a theoretical basis for the design of discharge devices and catalysts in the plasma. N 2 false( normalv false) + O • → NO + N • O 2 false( normalv false) + N • → NO + O • N • + OH → NO + H • …”

Section: Introductionmentioning

confidence: 99%

Insights on the Mechanism of Surface-Catalyzed Oxidative Nitrogen Fixation Based on Liquid-Phase Bubble Pin-Plate Discharge

Wang,

Liu,

Gao

et al. 2024

ACS Catal.

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In plasma-coupled catalytic oxidation of nitrogen fixation (NF), the gas−liquid phase combination and synergy with surface catalysis improve NF conversion and reduce energy consumption. However, there is a lack of studies on the synergistic reaction mechanisms of plasma and surface catalysis. Therefore, this study designed a liquid-phase bubble pin-plate discharge device providing a ground electrode as a catalytic electrode for the study of catalytic coupled mechanisms and optimized the setup parameters. The NF performance of several metal materials was investigated as catalytic electrodes. Among them, Fe foils show the best performance, with a conversion of 1.08%, and Ni foils display the most limited performance. To further study the coupled mechanism, density functional theory calculations combined with the plasma diagnostic technique were used to reveal the corresponding reaction paths and decisive steps by calculating the energies of dissociation and adsorption of nitrogen-based reactive species on the surface of Fe and Ni foils and the energies of stepwise oxidation of N• radicals. The results show that the Eley−Rideal mechanism is the optimal mechanism for NF to NO and NO 2 , and the Fe foils are more favorable for the formation of adsorbed state N. These findings offer significant guidance for design of the reactor and catalysts for plasma-coupled catalytic NF.

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“…Herrmann et al [23] studied the influences of peak voltage and discharge gap distance on pulsed discharge behavior over the liquid surface. Gromov et al [24] reported the physical process at the gas-liquid interface in a single pulse mode and high-frequency burst. Xu et al [25] compared the pulsed discharge plasma and sinusoidal discharge plasma, the results showing that nanosecond pulsed discharge plasma has lower gas temperature and higher efficiency of bacterial inactivation in liquid than that of the sinusoidal discharge plasma.…”

Section: Introductionmentioning

confidence: 99%

Generation of High-Density Pulsed Gas–Liquid Discharge Plasma Using Floating Electrode Configuration at Atmospheric Pressure

Liu

Yuan

et al. 2022

Applied Sciences

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In this paper, a high-density gas–liquid discharge plasma is obtained combined with nanosecond pulse voltage and a floating electrode. The discharge images, the waveforms of pulse voltage and discharge current, and the optical emission spectra are recorded. Gas temperature and electron density are calculated by the optical emission spectra of N2 (C3Πu → B3Πg) and the Stark broadening of Hα, respectively. The emission intensities of N2 (C3Πu → B3Πg), N2+ (B2Σ → X2Π), OH (A2Σ → X2Π), O (3p5P → 3s5S0), He (3d3D → 3p3P20), gas temperature, and electron density are acquired by optical emission spectra to discuss plasma characteristics varying with spatial distribution, discharge gap, and gas flow rate. The spatial distributions of discharge characteristics, including gas temperature, electron density, and emission intensities of N2 (C3Πu → B3Πg), N2+ (B2Σ → X2Π), OH (A2Σ → X2Π), O (3p5P → 3s5S0), and He (3d3D → 3p3P20), are presented. It is found that a high-density discharge plasma with the electron density of 2.2 × 1015 cm−3 and low gas temperature close to room temperature is generated. While setting the discharge gap distance at 10 mm, the discharge area over liquid surface has the largest diameter of 20 mm; under the same conditions, electron density is in the order of 1015 cm−3, and gas temperature is approximately 330 K. In addition, the discharge plasma characteristics are not kept consistent in the axial direction, in which the emission intensities of N2+ (B2Σ → X2Π), N2 (C3Πu → B3Πg), OH (A2Σ → X2Π), and gas temperature increased near the liquid surface. As the discharge gap is enlarged, the gas temperature increases, whereas the electron density remains almost constant. Moreover, as the gas flow rate was turned up, the electron density increased and the gas temperature was kept constant at 320 K.

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Plasma nitrogen fixation in the presence of a liquid interface: role of OH radicals

Abstract: Physical backgrounds of nitrogen fixation process in a nanosecond pulsed discharge in the presence of a plasma/liquid interface are reported. The role of OH radicals and O atoms in NO...

Cited by 6 publications

References 21 publications

Plasma‐Assisted Sustainable Nitrogen‐to‐Ammonia Fixation: Mixed‐phase, Synergistic Processes and Mechanisms

Plasma‐Assisted Sustainable Nitrogen‐to‐Ammonia Fixation: Mixed‐phase, Synergistic Processes and Mechanisms

Insights on the Mechanism of Surface-Catalyzed Oxidative Nitrogen Fixation Based on Liquid-Phase Bubble Pin-Plate Discharge

Generation of High-Density Pulsed Gas–Liquid Discharge Plasma Using Floating Electrode Configuration at Atmospheric Pressure

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