Sustainability analysis of methane-to-hydrogen-to-ammonia conversion by integration of high-temperature plasma and non-thermal plasma processes

Osorio-Tejada, José Luis; Veer, Kevin van’t; Long, Nguyen Van Duc; Tran, Nam Nghiep; Fulcheri, Laurent; Patil, Bhaskar; Bogaerts, Annemie; Hessel, Volker

doi:10.1016/j.enconman.2022.116095

Cited by 22 publications

(10 citation statements)

References 67 publications

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“…A direct comparison of plasma to conventional processes has yet to be explored as the former technology is still in its infancy and optimization and scaling of such processes are yet to be investigated. Techno-economic analysis (TEA) and life cycle assessment (LCA) conducted with other plasma processes, such as methanol, ethane, and ammonia production, − show that the demand for electricity is the main driving cost for all plasma-assisted processes . In the plasma oxidation process of n -alkanes, the cost of separation will need to be accounted for; however, by optimizing the process for high power and short treatment time, a high energy yield and selectivity can be achieved to reduce separation and electrical costs.…”

Section: Resultsmentioning

confidence: 99%

Oxidative Functionalization of Long-Chain Liquid Alkanes by Pulsed Plasma Discharges at Atmospheric Pressure

Nguyen

Dimitrakellis

Talley

et al. 2022

ACS Sustainable Chem. Eng.

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We introduce the oxidation of long aliphatic alkanes using non-thermal, atmospheric plasma processing as an eco-friendly route for organic synthesis. A pulsed dielectric barrier discharge in He/O2 gas mixtures was employed to functionalize n-octadecane. C18 secondary alcohols and ketones were the main products, with an optimal molar yield of ∼29.2%. Prolonged treatment resulted in the formation of dialcohols, diketones, and higher molecular weight oxygenates. Lighter hydrocarbon products and decarboxylation to CO2 were also observed at longer treatment times and higher power inputs. A maximum energy yield of 5.48 × 10–8 mol/J was achieved at short treatment times and high powers, associated with higher selectivity to primary oxygenates. Direct hydroxylation of alkyl radicals, as well as disproportionation reactions, are proposed as the main pathways to alcohols and ketones. The results hold promise for functionalizing long hydrocarbon molecules at ambient conditions using catalyst-free plasma discharges.

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Section: Resultsmentioning

confidence: 99%

Oxidative Functionalization of Long-Chain Liquid Alkanes by Pulsed Plasma Discharges at Atmospheric Pressure

Nguyen

Dimitrakellis

Talley

et al. 2022

ACS Sustainable Chem. Eng.

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“…One of the variables is the possibility of offshore NH 3 production, and this approach leads to an estimated cost of 1556–1670 $ per ton. Osorio-Tejada et al 56 reported that 2.2 mol% NH 3 yield and 1.1 g NH 3 kW −1 h −1 can be obtained at 302 °C, which is far from the present-day industry expectations. It was also mentioned that the plasma-catalytic method can be competitive if the cost of the plasma-catalytic ammonia synthesis falls below 452 $ per ton NH 3 .…”

Section: Challenges and Opportunitiesmentioning

confidence: 86%

Recent advances in plasma-enabled ammonia synthesis: state-of-the-art, challenges, and outlook

Zeng

Zhang

et al. 2023

Faraday Discuss.

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“…The recent ammonia production cost analyses by Wang et al [374] and Rouwenhorst et al [40,149] indicate that low outlet NH 3 , the recycling cost constitutes more than that of the ammonia synthesis cost for a distributed production platform. Therefore, several techniques have been adopted to enhance ammonia output concentration [3,39,40,148,149,375,376]. Evidently, (see for example Table 15), this level of conversion (0.2%) used in the model is too low.…”

Section: Conclusion and Recommendationsmentioning

confidence: 99%

Hydrogen, Ammonia and Symbiotic/Smart Fertilizer Production Using Renewable Feedstock and CO2 Utilization through Catalytic Processes and Nonthermal Plasma with Novel Catalysts and In Situ Reactive Separation: A Roadmap for Sustainable and Innovation-Based Technology

Akay

2023

Catalysts

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This multi-disciplinary paper aims to provide a roadmap for the development of an integrated, process-intensified technology for the production of H2, NH3 and NH3-based symbiotic/smart fertilizers (referred to as target products) from renewable feedstock with CO2 sequestration and utilization while addressing environmental issues relating to the emerging Food, Energy and Water shortages as a result of global warming. The paper also discloses several novel processes, reactors and catalysts. In addition to the process intensification character of the processes used and reactors designed in this study, they also deliver novel or superior products so as to lower both capital and processing costs. The critical elements of the proposed technology in the sustainable production of the target products are examined under three-sections: (1) Materials: They include natural or synthetic porous water absorbents for NH3 sequestration and symbiotic and smart fertilizers (S-fertilizers), synthesis of plasma interactive supported catalysts including supported piezoelectric catalysts, supported high-entropy catalysts, plasma generating-chemical looping and natural catalysts and catalysts based on quantum effects in plasma. Their performance in NH3 synthesis and CO2 conversion to CO as well as the direct conversion of syngas to NH3 and NH3—fertilizers are evaluated, and their mechanisms investigated. The plasma-generating chemical-looping catalysts (Catalysts, 2020, 10, 152; and 2016, 6, 80) were further modified to obtain a highly active piezoelectric catalyst with high levels of chemical and morphological heterogeneity. In particular, the mechanism of structure formation in the catalysts BaTi1−rMrO3−x−y{#}xNz and M3O4−x−y{#}xNz/Si = X was studied. Here, z = 2y/3, {#} represents an oxygen vacancy and M is a transition metal catalyst. (2) Intensified processes: They include, multi-oxidant (air, oxygen, CO2 and water) fueled catalytic biomass/waste gasification for the generation of hydrogen-enriched syngas (H2, CO, CO2, CH4, N2); plasma enhanced syngas cleaning with ca. 99% tar removal; direct syngas-to-NH3 based fertilizer conversion using catalytic plasma with CO2 sequestration and microwave energized packed bed flow reactors with in situ reactive separation; CO2 conversion to CO with BaTiO3−x{#}x or biochar to achieve in situ O2 sequestration leading to higher CO2 conversion, biochar upgrading for agricultural applications; NH3 sequestration with CO2 and urea synthesis. (3) Reactors: Several patented process-intensified novel reactors were described and utilized. They are all based on the Multi-Reaction Zone Reactor (M-RZR) concept and include, a multi-oxidant gasifier, syngas cleaning reactor, NH3 and fertilizer production reactors with in situ NH3 sequestration with mineral acids or CO2. The approach adopted for the design of the critical reactors is to use the critical materials (including natural catalysts and soil additives) in order to enhance intensified H2 and NH3 production. Ultimately, they become an essential part of the S-fertilizer system, providing efficient fertilizer use and enhanced crop yield, especially under water and nutrient stress. These critical processes and reactors are based on a process intensification philosophy where critical materials are utilized in the acceleration of the reactions including NH3 production and carbon dioxide reduction. When compared with the current NH3 production technology (Haber–Bosch process), the proposed technology achieves higher ammonia conversion at much lower temperatures and atmospheric pressure while eliminating the costly NH3 separation process through in situ reactive separation, which results in the production of S-fertilizers or H2 or urea precursor (ammonium carbamate). As such, the cost of NH3-based S-fertilizers can become competitive with small-scale distributed production platforms compared with the Haber–Bosch fertilizers.

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Sustainability analysis of methane-to-hydrogen-to-ammonia conversion by integration of high-temperature plasma and non-thermal plasma processes

Cited by 22 publications

References 67 publications

Oxidative Functionalization of Long-Chain Liquid Alkanes by Pulsed Plasma Discharges at Atmospheric Pressure

Oxidative Functionalization of Long-Chain Liquid Alkanes by Pulsed Plasma Discharges at Atmospheric Pressure

Recent advances in plasma-enabled ammonia synthesis: state-of-the-art, challenges, and outlook

Hydrogen, Ammonia and Symbiotic/Smart Fertilizer Production Using Renewable Feedstock and CO2 Utilization through Catalytic Processes and Nonthermal Plasma with Novel Catalysts and In Situ Reactive Separation: A Roadmap for Sustainable and Innovation-Based Technology

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