Identifying Regimes During Plasma Catalytic Ammonia Synthesis

Gershman, Sophia; Fetsch, Henry; Gorky, Fnu; Carreon, Maria L.

doi:10.1007/s11090-022-10258-y

Cited by 24 publications

(21 citation statements)

References 68 publications

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“…A sample OES broad spectrum for silica packing is provided as Figure S4 in the Supporting Information. The presence of the N 2 (C 3 Π u → B 3 Π g ) second positive system and the weak band of N 2 (B 3 Π g → A 3 Π u ) first positive systems shows that N 2 molecules are electronically excited by electrons in the plasma: e + N 2 → e + N 2 *. , Observation of the N 2 + first negative system with peaks at 391.2 and 427 nm confirms electron-impact ionization of N 2 molecules in the plasma: e + N 2 → 2e + N 2 + . , The hydrogen Balmer lines, with H β at 486.2 nm − and H α at 656 nm, , indicate that atomic H was present in the plasma. These hydrogen Balmer lines have been extensively used in atmospheric pressure plasma for density calculation using stark broadening. − The existence of atomic N species in the plasma was confirmed by emission lines at several wavelengths: 742, 818.5, 822, 824, 939, and 1011 nm .…”

Section: Resultsmentioning

confidence: 91%

“…54,55 Observation of the N 2 + first negative system with peaks at 391.2 and 427 nm confirms electronimpact ionization of N 2 molecules in the plasma: e + N 2 → 2e + N 2 + . 17, 54 The hydrogen Balmer lines, with H β at 486.2 nm 56−58 and H α at 656 nm, 46,59 indicate that atomic H was present in the plasma. These hydrogen Balmer lines have been extensively used in atmospheric pressure plasma for density calculation using stark broadening.…”

Section: Oes Spectra Andmentioning

confidence: 99%

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Effect of Porous Catalyst Support on Plasma-Assisted Catalysis for Ammonia Synthesis

et al. 2022

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We report on the effect of catalyst support particle porosity on the conversion of NH3 synthesis from N2 and H2 in a coaxial dielectric barrier discharge (DBD) plasma reactor. The discharge was created using an AC applied voltage with the reactor at room temperature and near atmospheric pressure (550 Torr). Two different particles of almost equal diameter (∼1.5 mm)porous silica (SiO2) ceramic beads (average pore size: 8 nm) and smooth, nonporous soda lime glass beadswere compared in the DBD reactor. As the pore size in the SiO2 particles was smaller than the Debye length, penetration of the plasma into the pores of the particles was unlikely; however, reactive species generated in the plasma outside the particles could diffuse into the pores. The N2 conversion and energy yield of NH3 increased with applied voltage for both particle types, and these values were consistently higher when using the SiO2 beads. Discharge and plasma properties were estimated from Lissajous plots and using calculations with the BOLSIG+ software. The effect of these two different catalyst supports on the physical properties of the discharge was negligible. High resolution optical emission spectra revealed that the concentrations of N2 +, atomic N, and atomic H (Hα, Hβ) in the plasma discharge were lower with the porous SiO2 beads than with the glass beads at every applied voltage tested. This indicates that these active species participate in heterogeneous reactions at support particle surfaces and that the larger surface area presented by the porous particles led to higher rates of depletion of these intermediates and a higher rate of ammonia synthesis.

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Section: Resultsmentioning

confidence: 91%

Section: Oes Spectra Andmentioning

confidence: 99%

Effect of Porous Catalyst Support on Plasma-Assisted Catalysis for Ammonia Synthesis

et al. 2022

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“…26 Indeed, our group has studied ammonia synthesis over NTP catalytic processes over the past years. [27][28][29][30][31][32] The achieved fundamental understanding on the effects of different catalysts, plasma-catalyst synergisms, and energy efficiency on ammonia synthesis allow us to primarily estimate the great potential of ammonia synthesis from N2 and "green" H2 sources, which is an important step to achieve zero-carbon ammonia synthesis. In fact, Zhou and co-workers are pioneers 33,34 to substitute H2 by water for plasma-assisted ammonia synthesis over a notable supported Ru catalyst and obtain an ammonia synthesis rate of around 2.7 mmol.gcat -1 .h -1 .…”

Section: Introductionmentioning

confidence: 99%

“…Our catalyst selection is supported by our group's previous experience on rational design of catalysts for ammonia synthesis. 27,30,39 Moreover, it has been indicated that silica-based catalysts promote the decomposition of N2O, 40,41 which is an unwanted by-product during ammonia production from water and N2. 33 Given its wide availability, seawater is the most sustainable replacement for hydrogen in ammonia synthesis powered by NTP.…”

Section: Introductionmentioning

confidence: 99%

Sustainable ammonia synthesis from seawater and nitrogen by single-step plasma catalysis: a step towards New England’s farmers nitrogen autonomy

Gorky

Guthrie

Carreon

2022

Preprint

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Ammonia synthesis at ambient conditions employing intermittent green sources of energy and feedstocks is globally sought to replace the Haber-Bosch (H-B) process operating at high temperature and pressure. We report herein for the first time an effective and sustainable ammonia synthesis pathway from seawater and N2 over a spherical SiO2 and M/SiO2 (M: Ag, Cu, and Co) catalysts driven by non-thermal plasma (NTP). Experimental results indicate that the presence of a catalyst is required for ammonia production from seawater and N2. The Co/SiO2 catalyst delivered the highest ammonia synthesis rate (rate NH3) of 3.7 mmol.gcat-1.h-1 and energy yield of 3.2 g-NH3.kWh-1 at a relatively low input power of 2 W. The extraction of H atom from H2O (seawater) molecules plays an important role in the ammonia synthesis from seawater. This work unfolds a novel platform for the subsequent optimization of sustainable ammonia production from endless resources such as seawater and N2 through catalytic non-thermal plasma potentially powered by renewable sources.

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“…This added to their conceptualization as modular small-scale systems for ammonia synthesis results in simple lightweight units compared to high pressure thermal reactors, which comprise added complex insulation/cooling systems [26]. Indeed, our group has studied ammonia synthesis over NTP catalytic processes over the past years [27][28][29][30][31][32]. The achieved fundamental understanding on the effects of different catalysts, plasma-catalyst synergisms, and energy efficiency on ammonia synthesis allow us to primarily estimate the great potential of ammonia synthesis from N2 and "green" H2 sources, which is an important step to achieve zero-carbon ammonia synthesis.…”

Section: Introductionmentioning

confidence: 99%

Sustainable ammonia synthesis from nitrogen wet with sea water vapor by single-step plasma catalysis

Gorky

Guthrie

Carreon

2022

Preprint

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Ammonia synthesis at ambient conditions employing intermittent distributed green sources of energy and feedstocks is globally sought to replace the centralized Haber-Bosch (H-B) process operating at high temperature and pressure. We report herein for the first time an effective and sustainable ammonia synthesis pathway from N2 wet with seawater vapor over spherical SiO2 and M/SiO2 (M: Ag, Cu, and Co) catalysts driven by non-thermal plasma (NTP). Experimental results indicate that the presence of a catalyst is required for ammonia production from seawater vapor and N2. The Co/SiO2 catalyst delivered the highest ammonia synthesis rate rNH3 of 3.7 mmol.gcat-1.h-1 and energy yield of 3.2 g-NH3.kW-1.h-1 at a relatively low input power of 2 W. The extraction of H atoms from H2O molecules plays an important role in the ammonia synthesis from seawater vapor. This work unfolds a novel platform for the subsequent optimization of sustainable ammonia production from endless resources such as seawater and N2 through catalytic non-thermal plasma potentially powered by renewable sources.

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Identifying Regimes During Plasma Catalytic Ammonia Synthesis

Cited by 24 publications

References 68 publications

Effect of Porous Catalyst Support on Plasma-Assisted Catalysis for Ammonia Synthesis

Effect of Porous Catalyst Support on Plasma-Assisted Catalysis for Ammonia Synthesis

Sustainable ammonia synthesis from seawater and nitrogen by single-step plasma catalysis: a step towards New England’s farmers nitrogen autonomy

Sustainable ammonia synthesis from nitrogen wet with sea water vapor by single-step plasma catalysis

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