Exploring the sustainable production of ammonia by recycling N and H in biological residues: Evolution of fuel-N during glutamic acid gasification

Gil-Lalaguna, Noemí; Afailal, Zainab; Aznar, María Pilar Matud; Fonts, Ìsabel

doi:10.1016/j.jclepro.2020.124417

Cited by 21 publications

(11 citation statements)

References 57 publications

(110 reference statements)

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“…Ammonia is the second most produced chemical in the world . It is synthesized from H 2 and N 2 via the Haber–Bosch process, accounting for about 2% of the worldwide fossil energy use. , Considerable amounts of fixed nitrogen are contained within biomass that could be recycled to ammonia via gasification and reduction. , The transformation from NO/NO 2 – to ammonia has been shown to be efficiently carried out using iron and cobalt porphyrin complexes − and occurs via a series of proton/electron transfer events.…”

Section: Introductionmentioning

confidence: 99%

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]⁺-Based Protic Ionic Liquid Nanodomains

2021

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The reduction of [Fe(OEP)(NO)] has been studied in the presence of aprotic room-temperature ionic liquids (RTIL) and protic (PIL) ionic liquids dissolved within a molecular solvent (MS). The cyclic voltammetric results showed the formation of RTIL nanodomains at low concentrations of the RTIL/PIL solutions. The pK a values of the two PILs studied (i.e., trialkylammonium and [DBU−H] + -based ionic liquids) differed by four units in THF. While voltammetry in solutions containing all three RTILs showed similar potential shifts of the first reduction of [Fe(OEP)(NO)] to [Fe(OEP)(NO)] − at low concentrations, significant differences were observed at higher concentrations for the ammonium PIL. The trialkylammonium cation had previously been shown to protonate the {FeNO} 8 species at room temperature. Visible and infrared spectroelectrochemistry revealed that the [DBU−H] + -based PIL formed hydrogen bonds with [Fe(OEP)(NO)] − rather than formally protonating it. Despite these differences, both PILs were able to efficiently reduce the nitrosyl species to the hydroxylamine complex, which could be further reduced to ammonia. On the voltammetric time scale and when the switching potential was positive of the Fe(II)/Fe(I) potential, the hydroxylamine complex was re-oxidized back to the NO complex via direct oxidation of the coordinated hydroxylamine at low scan rates or initial oxidation of the ferrous porphyrin at high scan rates. The results of this work show that, while [DBU−H] + does not protonate electrochemically generated [Fe(OEP)(NO)] − , it still plays an important role in efficiently reducing the nitroxyl ligand via a series of proton-coupled electron transfer steps to generate hydroxylamine and eventually ammonia. The overall reaction rates were independent of the PIL concentration, consistent with the nanodomain formation being important to the reduction process.

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Section: Introductionmentioning

confidence: 99%

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]⁺-Based Protic Ionic Liquid Nanodomains

2021

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“…Inspired by the utilization of biomass as a carbon source for the synthesis of chemicals and fuel, nitrogenenriched biomass is capable of being a sustainable source of renewable nitrogen and hydrogen to fulfill the growing demand for the production of ammonia. 15,16 Pyrolysis and gasification offer an efficient pathway for converting fuel-N into ammonia. 17,18 To this end, ammonia production from nitrogen-enriched biomass pyrolysis/gasification offers an innovative alternative that treats nitrogen-enriched biomass as a hydrogen-and nitrogen-rich resource to generate ammonia under ambient pressure.…”

Section: Introductionmentioning

confidence: 99%

Exploring the Green Production of Ammonia from Nitrogen-Enriched Biowaste Gasification: Nitrogen Conversion from Tea Waste and Theanine

Wang,

Xu,

Shen

et al. 2023

Ind. Eng. Chem. Res.

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“…It is a potential alternative route to obtain ammonia from nitrogen-rich biomass. 13,14 Each year, huge amounts of biomass with a high nitrogen content, such as sewage sludge, 15 microalgae, 16 and mycelial waste, 17 are produced. These nitrogen-rich biomasses might be a potential sustainable supply source of nitrogen and hydrogen.…”

Section: Introductionmentioning

confidence: 99%

“…These nitrogen-rich biomasses might be a potential sustainable supply source of nitrogen and hydrogen. 13,18 Pyrolysis, one of the useful techniques for valorization of biomass, refers to the thermal decomposition of substances by heating in the absence of oxygen, in which biomass can be converted into multiple products (char, tar, and gas). During pyrolysis, the intrinsic nitrogen in biomass (fuel−N) is finally transformed into char−N, tar−N, and gas−N.…”

Section: Introductionmentioning

confidence: 99%

“…It is a potential alternative route to obtain ammonia from nitrogen-rich biomass. , Each year, huge amounts of biomass with a high nitrogen content, such as sewage sludge, microalgae, and mycelial waste, are produced. These nitrogen-rich biomasses might be a potential sustainable supply source of nitrogen and hydrogen. , Pyrolysis, one of the useful techniques for valorization of biomass, refers to the thermal decomposition of substances by heating in the absence of oxygen, in which biomass can be converted into multiple products (char, tar, and gas). During pyrolysis, the intrinsic nitrogen in biomass (fuel–N) is finally transformed into char–N, tar–N, and gas–N .…”

Section: Introductionmentioning

confidence: 99%

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Fast Pyrolysis of Tea Waste under a Hydrogen-Rich Atmosphere: A Study on Nitrogen Evolution and Green Ammonia Production

Wang

Shen

2022

Energy Fuels

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Nitrogen-rich biomass pyrolysis has been explored as a green, distributed, and simple alternative for sustainable ammonia production at atmospheric pressure. In this paper, tea waste was selected as a promising feedstock, and H 2 was employed as an enhancer to increase the yield of NH 3 . The nitrogen distribution among three-phase pyrolytic products affected by various temperatures and different atmospheres was compared and discussed. The evolution pathways for fuel−N during tea waste pyrolysis under a H 2 -rich atmosphere were concluded. Results indicated that the introduction of H 2 was favorable for the increase of the gas− N yield but decreased the yields of char−N and tar−N. At lower temperatures, the bond cleavage of amide−N (N−A) in fuels was enhanced by H 2 , which then yielded more NH 3 −N through deamination. Subsequently, H 2 improved the production of nitrile−N in tar, as well as NH 3 −N and HCN−N, by accelerating the secondary cracking of amine−N (tar−N) generated from the decomposition of amide−N. However, the formation of heterocyclic−N in tar through the polymerization of amine−N was restrained under a H 2 -rich atmosphere. Pyrolysis in the presence of H 2 generated a large amount of H radicals. When the temperature continued to increase, sufficient H radicals impressively advanced the ring rupture (into HCN−N) and full hydrogenation (into NH 3 −N) of pyridinic−N/pyrrolic−N (N-6/N-5) in char. Meanwhile, H radicals also intensified the thermal cracking of nitrile−N and ring opening of heterocyclic−N to form more HCN−N and NH 3 −N. Overall, more nitrogen evolved into NH 3 −N and HCN−N during pyrolysis in a H 2 -rich atmosphere, especially at high temperatures. The highest NH 3 yield of 43.33 wt % was achieved at 800 °C under a 25% H 2 + 75% Ar atmosphere.

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Exploring the sustainable production of ammonia by recycling N and H in biological residues: Evolution of fuel-N during glutamic acid gasification

Cited by 21 publications

References 57 publications

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]⁺-Based Protic Ionic Liquid Nanodomains

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]⁺-Based Protic Ionic Liquid Nanodomains

Exploring the Green Production of Ammonia from Nitrogen-Enriched Biowaste Gasification: Nitrogen Conversion from Tea Waste and Theanine

Fast Pyrolysis of Tea Waste under a Hydrogen-Rich Atmosphere: A Study on Nitrogen Evolution and Green Ammonia Production

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Exploring the sustainable production of ammonia by recycling N and H in biological residues: Evolution of fuel-N during glutamic acid gasification

Cited by 21 publications

References 57 publications

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]+-Based Protic Ionic Liquid Nanodomains

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]+-Based Protic Ionic Liquid Nanodomains

Exploring the Green Production of Ammonia from Nitrogen-Enriched Biowaste Gasification: Nitrogen Conversion from Tea Waste and Theanine

Fast Pyrolysis of Tea Waste under a Hydrogen-Rich Atmosphere: A Study on Nitrogen Evolution and Green Ammonia Production

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Product

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Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]⁺-Based Protic Ionic Liquid Nanodomains

Reversible Proton-Coupled Reduction of an Iron Nitrosyl Porphyrin within [DBU–H]⁺-Based Protic Ionic Liquid Nanodomains