Electrified chemical reactors for methane-to-ethylene conversion

Delikonstantis, Evangelos; Cameli, Fabio; Stefanidis, Georgios D.

doi:10.1016/j.coche.2023.100927

Cited by 4 publications

(4 citation statements)

References 51 publications

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“…Although there are no references in the literature so far, electrified (Joule-heated) reactors can conceptually be used to enable the thermocatalytic RWGS reaction simply by utilizing electricity for heating. If so, an electrified CAMERE process may emerge featuring also the characteristics the electrified reactors own . In this case, a technical benchmarking between the two electrified process alternatives, i.e., plasma (NPD)-assisted CAMERE process (concept developed in this work) and electrified CAMERE process (based on Joule-heated reactors), is of interest and presented in Table .…”

Section: Process Benchmarking and Assessmentmentioning

confidence: 99%

“…If so, an electrified CAMERE process may emerge featuring also the characteristics the electrified reactors own. 45 In this case, a technical benchmarking between the two electrified process alternatives, i.e., plasma (NPD)assisted CAMERE process (concept developed in this work) and electrified CAMERE process (based on Joule-heated reactors), is of interest and presented in Table 4.…”

Section: Process Benchmarking and Assessmentmentioning

confidence: 99%

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Valorizing the Steel Industry Off-Gases: Proof of Concept and Plantwide Design of an Electrified and Catalyst-Free Reverse Water–Gas-Shift-Based Route to Methanol

Delikonstantis,

Vettas,

Cameli

et al. 2023

Environ. Sci. Technol.

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Conversion of steel industry off-gases to value-added chemicals enabled by renewable electricity can significantly reduce the environmental burden of the steelmaking process. Herein, we demonstrate that CO2 reduction by H2, both contained in steel mill off-gases, to form syngas via the reverse water–gas-shift reaction is effectively performed by nanosecond pulsed discharges at atmospheric pressure. The experimental results suggest the following: (i) An optimum interelectrode distance exists, maximizing CO2 conversion. (ii) CO2 conversion at constant SEI follows a nonmonotonic trend with H2 excess. CO2 conversion increases with H2 excess up to H2:CO2 = 3:1 upon shifting the chemical equilibrium. At larger H2:CO2, both gas cooling, promoted by the high H2 content, and hindered CO2 collisions in a highly diluted stream hamper CO2 conversion. (iii) SEI enhances CO2 conversion, but the effect decreases with increasing SEI due to equilibrium limitations. A stoichiometric H2:CO2 feed ratio in the plasma reactor is recommended for higher energy efficiency. Intensifying MeOH productivity via SEI elevation is not advised as a 2-fold SEI increase results only in 17% higher MeOH throughput.

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Section: Process Benchmarking and Assessmentmentioning

confidence: 99%

Section: Process Benchmarking and Assessmentmentioning

confidence: 99%

Valorizing the Steel Industry Off-Gases: Proof of Concept and Plantwide Design of an Electrified and Catalyst-Free Reverse Water–Gas-Shift-Based Route to Methanol

Delikonstantis,

Vettas,

Cameli

et al. 2023

Environ. Sci. Technol.

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Section: Introductionmentioning

confidence: 99%

“…The chemical industry’s defossilation requires the electrification of highly endothermic reactions ( 8 ). Nonthermal plasma, dielectric and Joule heating, and plasmonic photocatalysis are such emerging technologies ( 8 , 9 ). Nonthermal plasma is a gas where excited species, radicals, ions, and neutral molecules at near ambient temperatures ( T g ≤ 10 3 K) coexist with high-energy electrons at temperatures ( T e ≥ 10 4 K) ( 10 ).…”

Section: Introductionmentioning

confidence: 99%

Direct HCN synthesis via plasma-assisted conversion of methane and nitrogen

Kamarinopoulou,

Wittreich,

Vlachos

2024

Sci. Adv.

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Hydrogen cyanide (HCN) is synthesized from ammonia (NH 3 ) and methane (CH 4 ) at ~ 1200°C over a Pt catalyst. Ammonia synthesis entails several complex, highly emitting processes. Plasma-assisted HCN synthesis directly from CH 4 and nitrogen (N 2 ) could be pivotal for on-demand HCN production. Here, we evaluate the potential of dielectric barrier discharge (DBD) N 2 /CH 4 plasma for decentralized catalyst-free selective HCN production. We demonstrate a single-step conversion of methane and nitrogen to HCN with a 72% yield at <300°C. HCN is favored at low CH 4 concentrations with ethane (C 2 H 6 ) as the secondary product. We propose a first-principles microkinetic model with few electron impact reactions. The model accurately predicts primary product yields and elucidates that methyl radical (·CH 3 ) is a common intermediate in HCN and C 2 H 6 synthesis. Compared to current industrial processes, N 2 /CH 4 DBD plasma can achieve minimal CO 2 emissions.

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