Understanding plasma-assisted ammonia synthesis via crossing discipline borders of literature: A critical review

Long, Nguyen Van Duc; Al-Bared, Mohamad; Lin, Liangliang; Davey, K. G.; Tran, Nam Nghiep; Pourali, Nima; Ostrikov, Kostya; Rebrov, Evgeny V.; Hessel, Volker

doi:10.1016/j.ces.2022.118097

Cited by 14 publications

(5 citation statements)

References 71 publications

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“…This means the resulting corrected data in Figure are representative of the NH and NO ground state concentrations in the plasma. It has been shown that NH is predictive of and correlates with the concentration of NH 3 . In (humid) N 2 , the trend of NO(A 2 Σ + ) intensity follows the gas phase HNO 2 concentration with increasing H 2 O content, suggesting NO is directly involved in HNO 2 formation (Figure a,b).…”

Section: Resultsmentioning

confidence: 99%

NH₃and HNO_xFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

Vervloessem

Gromov

Bogaerts

et al. 2023

ACS Sustainable Chem. Eng.

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The current global energy crisis indicated that increasing our insight into nonfossil fuel nitrogen fixation pathways for synthetic fertilizer production is more crucial than ever. Nonequilibrium plasma is a good candidate because it can use N2 or air as a N source and water directly as a H source, instead of H2 or fossil fuel (CH4). In this work, we investigate NH3 gas phase formation pathways from humid N2 and especially humid air up to 2.4 mol % H2O (100% relative humidity at 20 °C) by optical emission spectroscopy and Fourier-transform infrared spectroscopy. We demonstrate that the nitrogen fixation capacity is increased when water vapor is added, as this enables HNO2 and NH3 production in both N2 and air. However, we identified a significant loss mechanism for NH3 and HNO2 that occurs in systems where these species are synthesized simultaneously; i.e., downstream from the plasma, HNO2 reacts with NH3 to form NH4NO2, which rapidly decomposes into N2 and H2O. We also discuss approaches to prevent this loss mechanism, as it reduces the effective nitrogen fixation when not properly addressed and therefore should be considered in future works aimed at optimizing plasma-based N2 fixation. In-line removal of HNO2 or direct solvation in liquid are two proposed strategies to suppress this loss mechanism. Indeed, using liquid H2O is beneficial for accumulation of the N2 fixation products. Finally, in humid air, we also produce NH4NO3, from the reaction of HNO3 with NH3, which is of direct interest for fertilizer application.

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Section: Resultsmentioning

confidence: 99%

NH₃and HNO_xFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

Vervloessem

Gromov

Bogaerts

et al. 2023

ACS Sustainable Chem. Eng.

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“…As shown in an exemplary OES spectrum (Figure S5), prominent N 2 spectral bands (310−410 nm) and Ar atomic lines (690− 850 nm) together with less intensive CH lines were observed, suggesting the presence of energetic species. 41 On the other hand, the detailed interactions between the plasma and polymers were not clear since plasma polymerization is a complex process in which monomers are cross-linked, fragmented, or rearranged to form irregularly structured polymers rather than polymers with repetitive units.…”

Section: Resultsmentioning

confidence: 99%

Fluorescent Patterning of Polymeric Substrates with Rare-Earth-Doped Nanophosphors Assisted by Atmospheric Pressure Plasma

Rui,

Li,

et al. 2023

Ind. Eng. Chem. Res.

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The direct, efficient, and controllable patterning of fluorescent materials on polymers is crucial for fundamental research and industrial application but very challenging. Herein, a DBD plasma method was used to deposit rare-earth-doped nanophosphors on the surface of polymeric substrates without thermal annealing steps, aiming to realize fluorescent patterning of thermally sensitive polymers through a simple and low-temperature process. Eu- and Tb-doped yttria (Y2O3) nanoparticles of different fluorescence properties were synthesized from rare-earth acetylacetonates to verify the feasibility of the process, followed by the formation of desirable fluorescent patterns on poly(vinylidene difluoride) (PVDF) membranes using relief printing to demonstrate the flexibility of this novel strategy. The results showed that crystalline rare-earth-doped Y2O3 nanophosphors were rapidly generated in plasma and can be deposited on the PVDF membranes to form fluorescent patterns without damaging the polymeric substrates. This method was further expanded to diverse substrates like polypropylene (PP), polyether sulfone (PES), and nylon, revealing the versatility of direct fluorescent patterning on thermally sensitive polymers. The efficient, flexible, and rapid plasma process combined with the desirable high-fluorescence patterns is expected to supply guidance for the design and fabrication of functional polymers.

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“…Emission peaks could be observed in the range 200-1000 nm, which allowed to identify excited species contained in the gas phase (Figure 2a). The different identified peaks are located at 315 nm (N 2 * C 3 Q u !B 3 Q g 1-0), [22] 336 nm and 337 nm (NH°biradicals and N 2 * C 3 Q u !B 3 Q g 0-0, respectively), [22][23][24][25][26] at 357 nm (N 2 * C 3 Q !B 3 Q 0-1) [22,23,25,26] and 380 nm (N 2 * C 3 Q u !B 3 Q g 0-2). [22] This analysis confirmed the dissociation of ammonia in the plasma with the formation of NH°and excited neutrals N 2 *.…”

Section: Results and Discussion Characterization Of The Plasmamentioning

confidence: 99%

Direct Amination of Benzene with Ammonia by Flow Plasma Chemistry

Dupont

Ognier

Morand

et al. 2023

Chemistry A European J

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Amine derivatives, including aniline and allylic amines, can be formed in a single‐step process from benzene and an ammonia plasma in a micro‐reactor. Different process parameters such as temperature, residence time, and plasma power were evaluated to improve the reaction yield and its selectivity toward aminated products and avoid hydrogenated or oligomerized products. In parallel, simulation studies of the process have been carried out to propose a global mechanism and gain a better understanding of the influence of the different process parameters. The exploration of diverse related alkenes showed that the double bonds, conjugation, and aromatization influenced the amination mechanism. Benzene was the best reactant for amination based on the lifetime of radical intermediates. Under optimized conditions, benzene was aminated in the absence of catalyst with a yield of 3.8% and a selectivity of 49% in various amino compounds,

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Understanding plasma-assisted ammonia synthesis via crossing discipline borders of literature: A critical review

Cited by 14 publications

References 71 publications

NH₃and HNO_xFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

NH₃and HNO_xFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

Fluorescent Patterning of Polymeric Substrates with Rare-Earth-Doped Nanophosphors Assisted by Atmospheric Pressure Plasma

Direct Amination of Benzene with Ammonia by Flow Plasma Chemistry

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Understanding plasma-assisted ammonia synthesis via crossing discipline borders of literature: A critical review

Cited by 14 publications

References 71 publications

NH3and HNOxFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

NH3and HNOxFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

Fluorescent Patterning of Polymeric Substrates with Rare-Earth-Doped Nanophosphors Assisted by Atmospheric Pressure Plasma

Direct Amination of Benzene with Ammonia by Flow Plasma Chemistry

Contact Info

Product

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About

NH₃and HNO_xFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma

NH₃and HNO_xFormation and Loss in Nitrogen Fixation from Air with Water Vapor by Nonequilibrium Plasma