Activation of two highly stable molecules – nitrogen and methane to co-produce ammonia and ethylene

Tiwari, Sarojini; Khan, Tuhin Suvra; Tavadze, Pedram; Hu, Jianli

doi:10.1016/j.cej.2020.127501

Cited by 9 publications

(6 citation statements)

References 47 publications

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“…Toward this goal, understanding the reaction mechanism is crucial for the development of highly efficient catalysts and larger-scale processes. Drawing from Tiwari et al [60] and Zhang et al [61] and adding from our own experiences in plasma-based CH 4 activation, we tender possible reactions pathways for producing ammonia and hydrocarbons from CH 4 and N 2 , as shown in Figure 3a, that should be followed as necessary and sufficient for further development of ammonia productions from CH 4 and N 2 . Typically, simultaneous activation of CH 4 and N 2 molecules involves two routes: (i) the dissociation to the chemisorption of CH 4 and N 2 molecules in both the plasma regime and the catalyst surface; and (ii) the formation of intermediates such as H*, N*, CH*, NH*, C x H y *, HCN*, and CN* followed by their combinations to final products.…”

Section: Improvements In Plasma-catalyst Synergymentioning

confidence: 99%

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Technical Challenges and Prospects in Sustainable Plasma Catalytic Ammonia Production from Methane and Nitrogen

M. Nguyen,

Omidkar,

Song

2023

ChemPlusChem

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Ammonia is crucial for human life as an important ingredient for fertilizer, industrial and household chemicals, and is considered as a future fuel alternative and hydrogen storage molecule. There remain no viable alternatives to the energy‐and capital‐intensive Haber–Bosch (H−B) process. Efforts in the development of novel catalytic processes operated at milder conditions (low temperatures and ambient pressure), prominently electrochemistry and non‐thermal plasma (NTP), and utilization of lower‐cost H sources for ammonia formation than the ultrapure H2 have been witnessed in the last few years. Yet, limited progress from these routes has been made to date given unresolved low ammonia yield and technical challenges. Several rare works attempted to activate methane (CH4) and nitrogen (N2) by non‐thermal plasma to produce ammonia and valued‐added hydrocarbons have proven to be a promising research direction, rivalling the reaction between N2 and ultrapure H2 or water. The direct conversion of CH4 and N2 to ammonia is still at the beginning level, and it remains unclear that what extent these technologies must be improved to develop a commercial process. Toward this goal, this Perspective critiques current steps and miss‐steps of sustainable plasma catalytic ammonia production from CH4 and N2 in terms of technology, plasma‐catalyst synergy, mechanistic insights, and experimental protocols. We discuss mechanistic understandings of catalyst‐promoted ammonia production and translate such discussions as well as key metrics achieved in the field into recommendations of feasible processes for ammonia and value‐added hydrocarbons formation from CH4 and N2.

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Section: Improvements In Plasma-catalyst Synergymentioning

confidence: 99%

“…Toward this goal, understanding the reaction mechanism is crucial for the development of highly efficient catalysts and larger‐scale processes. Drawing from Tiwari et al [60] . and Zhang et al [61] .…”

Section: Challenges and Prospects Of Plasma Catalytic Ammonia Product...mentioning

confidence: 99%

Technical Challenges and Prospects in Sustainable Plasma Catalytic Ammonia Production from Methane and Nitrogen

M. Nguyen,

Omidkar,

Song

2023

ChemPlusChem

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“…Tiwari et al reported that CH 4 and N 2 could be activated simultaneously over a K-doped Ru catalyst to co-produce ammonia and ethylene. 22 The in situ H 2 produced from CH 4 conversion was used as a hydrogen source for ammonia synthesis. However, coke is formed in parallel with hydrogen production, resulting in discontinuous ammonia productivity.…”

Section: Introductionmentioning

confidence: 99%

Co-activation of methane and nitrogen to acetonitrile over MoC_x/Al₂O₃ catalysts

Trangwachirachai¹,

Kao²,

Huang³

et al. 2023

Catal. Sci. Technol.

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“…Microwave is a cleaner and greener energy resource to drive the chemical reactions, and it has advantages in terms of extraordinary efficiency and high yield. The applications of microwave in chemical reactions are very wide, such as organic synthesis, − biomass treatment, − and nanomaterials. − Most accelerating chemical reactions under the microwave irradiation can be explained by the microwave thermal effect. , Numerous experimental studies determine that not only the microwave thermal effect but also the microwave nonthermal effect play a decisive role in enhancing chemical reactions. − Tiwari et al demonstrated the simultaneous activation of CH 4 and N 2 in a microwave catalytic reaction to produce NH 3 and C 2 products and found that the elementary reaction steps leading to NH 3 synthesis occurs due to the nonthermal effects of microwave irradiation. Silva et al verified that the combination of thermal and nonthermal effects during the microwave-assisted hydrothermal treatment provides ideal conditions for an efficient and rapid synthesis of pristine SrTiO 3 mesocrystals.…”

Section: Introductionmentioning

confidence: 99%

“…15,16 Numerous experimental studies determine that not only the microwave thermal effect but also the microwave nonthermal effect play a decisive role in enhancing chemical reactions. 17−41 Tiwari et al 22 demonstrated the simultaneous activation of CH 4 and N 2 in a microwave catalytic reaction to produce NH 3 and C 2 products and found that the elementary reaction steps leading to NH 3 synthesis occurs due to the nonthermal effects of microwave irradiation. Silva et al 26 verified that the combination of thermal and nonthermal effects during the microwave-assisted hydrothermal treatment provides ideal conditions for an efficient and rapid synthesis of pristine SrTiO 3 mesocrystals.…”

Section: Introductionmentioning

confidence: 99%

Investigation of Spatial Orientation and Kinetic Energy of Reactive Site Collision between Benzyl Chloride and Piperidine: Novel Insight into the Microwave Nonthermal Effect

et al. 2022

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Microwave nonthermal effect in chemical reactions is still an uncertain problem. In this work, we have studied the spatial orientation and kinetic energy of reactive site collision between benzyl chloride and piperidine molecules in substitution reaction under microwave irradiation using the molecular dynamics simulation. Our results showed that microwave polarization can change the spatial orientation of reactive site collision. Collision probability between the Cl atom of the C–Cl group of benzyl chloride and the H atom of the N–H group of piperidine increased by up to 33.5% at an effective spatial solid angle (θ, φ) of (100∼110°, 170∼190°) under microwave irradiation. Also, collision probability between the C atom of the C–Cl group of benzyl chloride and the N atom of the N–H group of piperidine also increased by up to 25.6% at an effective spatial solid angle (θ, φ) of (85∼95°, 170∼190°). Moreover, the kinetic energy of collision under microwave irradiation was also changed, that is, for the collision between the Cl atom of the C–Cl group and the H atom of the N–H group, the fraction of high-energy collision greater than 6.39 × 10–19 J increased by 45.9 times under microwave irradiation, and for the collision between the C atom of the C–Cl group and the N atom of the N–H group, the fraction of high-energy collision greater than 6.39 × 10–19 J also increased by 29.2 times. Through simulation, the reaction rate increased by 34.4∼50.3 times under microwave irradiation, which is close to the experimental increase of 46.3 times. In the end, spatial orientation and kinetic energy of molecular collision changed by microwave polarization are summarized as the microwave postpolarization effect. This effect provides a new insight into the physical mechanism of the microwave nonthermal effect.

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Activation of two highly stable molecules – nitrogen and methane to co-produce ammonia and ethylene

Cited by 9 publications

References 47 publications

Technical Challenges and Prospects in Sustainable Plasma Catalytic Ammonia Production from Methane and Nitrogen

Technical Challenges and Prospects in Sustainable Plasma Catalytic Ammonia Production from Methane and Nitrogen

Co-activation of methane and nitrogen to acetonitrile over MoC_x/Al₂O₃ catalysts

Investigation of Spatial Orientation and Kinetic Energy of Reactive Site Collision between Benzyl Chloride and Piperidine: Novel Insight into the Microwave Nonthermal Effect

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Activation of two highly stable molecules – nitrogen and methane to co-produce ammonia and ethylene

Cited by 9 publications

References 47 publications

Technical Challenges and Prospects in Sustainable Plasma Catalytic Ammonia Production from Methane and Nitrogen

Technical Challenges and Prospects in Sustainable Plasma Catalytic Ammonia Production from Methane and Nitrogen

Co-activation of methane and nitrogen to acetonitrile over MoCx/Al2O3 catalysts

Investigation of Spatial Orientation and Kinetic Energy of Reactive Site Collision between Benzyl Chloride and Piperidine: Novel Insight into the Microwave Nonthermal Effect

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Co-activation of methane and nitrogen to acetonitrile over MoC_x/Al₂O₃ catalysts