Selective Electrocatalytic Reduction of Nitrous Oxide to Dinitrogen with an Iron Porphyrin Complex

Stanley, Jared S.; Wang, Xinran S.; Yang, Jenny Y.

doi:10.1021/acscatal.3c02707

Cited by 12 publications

(8 citation statements)

References 35 publications

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“…In comparison with previous studies, the N 2 yield rate in this study was far more superior to those of the reported electrocatalytic N 2 O reduction ,, and Cu-based thermocatalytic N 2 O reduction ,− (Figure i). The unique structure of the SAC enables complete exposure of the active center, minimizing the quantity of metal required and resulting in a substantial cost reduction.…”

Section: Resultscontrasting

confidence: 75%

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High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Li,

Wu,

Wang

et al. 2024

Environ. Sci. Technol.

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Nitrous oxide (N 2 O) is a potent greenhouse gas with a high global warming potential, emphasizing the critical need to develop efficient elimination methods. Electrocatalytic N 2 O reduction reaction (N 2 ORR) stands out as a promising approach, offering room temperature conversion of N 2 O to N 2 without the production of NO x byproducts. In this study, we present the synthesis of a copper-based single-atom catalyst featuring atomic Cu on nitrogen-doped carbon black (Cu 1 −NCB). Attributed to the highly dispersed single-atom Cu sites and the effective suppression of the hydrogen evolution reaction, Cu 1 −NCB demonstrated an optimal N 2 faradaic efficiency (82.1%) and yield rate (3.53 mmol h −1 mg metal −1 ) at −0.2 and −0.5 V vs RHE, respectively, outperforming previously reported N 2 ORR electrocatalysts. Further, a gas diffusion electrode cell was employed to improve mass transfer and achieved a 28.6% conversion rate of 30% N 2 O with only a 14 s residence time, demonstrating the potential for practical application. Density functional theory calculations identified Cu−N 4 as the crucial active site for N 2 ORR, highlighting the significance of the unsaturated coordination and metal−support electronic structure. O-terminal adsorption of N 2 O was favored, and the dissociative adsorption (*ON 2 → *O + N 2 ) was the rate-determining step. These findings reveal the broad prospects of N 2 O decomposition via electrocatalysis.

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Section: Resultscontrasting

confidence: 75%

“…The recent upsurge in interest in N 2 ORR has prompted researchers to explore both homogeneous , and heterogeneous , catalysts for N 2 ORR. Homogeneous catalysts demonstrate exceptional metal atom utilization and adjustable catalytic activity; however, the challenge lies in the recovery of used catalysts.…”

Section: Introductionmentioning

confidence: 99%

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Li,

Wu,

Wang

et al. 2024

Environ. Sci. Technol.

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“…Nitrous oxide (N 2 O), also one of the chief greenhouse gases in the atmosphere, has strong radiation absorption capability, and its greenhouse effect potential is estimated to be around 300 times greater than that of CO 2 Moreover, N 2 O is the primary cause of ozone depletion, acid rain formation, and photochemical smog due to its long lifespan in the atmosphere. Human activities such as the artificial emission of industrial exhaust and the excessive use of chemical fertilizers in agriculture, as well as the growing demand for energy, have led to a sharp accrescence in N 2 O emissions in recent years .…”

Section: Introductionmentioning

confidence: 99%

Exploring the Micropore Functional Mechanism of N₂O Adsorption by the Eucalyptus Bark-based Porous Carbon

Mou,

Liu,

Gong

et al. 2024

Langmuir

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Nitrous oxide (N 2 O), recognized as a significant greenhouse gas, has received insufficient research attention in the past. In view of their low energy consumption and cost-effectiveness, the application of porous materials in adsorption is increasingly regarded as a potent strategy to reduce N 2 O pollution. In this study, a series of microporous porous carbons with a preeminent specific surface area (244.54−2018.08 m 2 g −1 ), which are derived from the fast-growing eucalyptus bark, were synthesized by KOH activation at high temperatures. The obtained materials demonstrated a relatively fine N 2 O capture capability (0.19− 0.68 mmol g −1 ) at normal temperature and pressure. More importantly, the optimal pore size affecting N 2 O adsorption (0.8 and 1.0 nm) has been detected, which is a meaningful view that has never been put forward in previous studies. The rationality of the N 2 O adsorption mechanism was also validated by combining the experimental analysis and Grand Canonical Monte Carlo (GCMC) simulation. The calculated results showed that 0.8 and 1.0 nm of the porous carbon were the preferred pore sizes for N 2 O adsorption, and the interaction force between N 2 O and the pore wall decreased with the increase of distance. This study provides a significant theoretical basis for the preparation of biomass porous carbon with excellent N 2 O adsorption performance and practical adsorption application.

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“…Iron tetraphenylporphyrins (TPPFe) are well-studied molecular catalysts for small molecule activation, in particular dioxygen reduction to water at the level of the formal Fe(III)/Fe(II) redox couple and carbon dioxide reduction to carbon monoxide at the level of the formal Fe(I)/Fe(0) redox couple, and even at the level of the Fe(II)/Fe(I) redox couple, provided an appropriate modification of the ligand environment is designed . Recently, TPPFe(0) has also been shown to trigger nitrous oxide reduction . All the latter activation reactions involve a deoxygenation process, usually assisted by protons, and likely generating hydroxide ions, known as ligands for iron porphyrins.…”

Section: Introductionmentioning

confidence: 99%

Redox Behavior and Kinetics of Hydroxo Ligand Exchange on Iron Tetraphenylporphyrin: Comparison with Chloro Exchange and Consequences for Its Role in Self-Modulation of Molecular Catalysis of Electrochemical Reactions

Chartier,

Chardon-Noblat,

Costentin

2024

Inorg. Chem.

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Thermodynamics and kinetics of hydroxide ion binding to iron tetraphenylporphyrin (TPPFe) at different redox states is investigated by electrochemistry and UV–vis spectroscopy. The reduction of initial TPPFe(III) drastically decreases the binding affinity of hydroxide ions. An activation-driving force correlation is revealed showing that the strongest the binding affinity, the largest the association rate constant and vice versa. Comparison with chloride ions shows that hydroxide ions are stronger ligands for iron tetraphenylporphyrin. However, kinetic data indicate that coordination and decoordination of chloride ions is intrinsically faster than coordination and decoordination of hydroxide ions. Finally, the consequence of hydroxide ion binding dynamics when TPPFe is used as a molecular catalyst for electrochemical reactions liberating hydroxides is discussed in the framework of self-modulation of catalytic processes.

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Selective Electrocatalytic Reduction of Nitrous Oxide to Dinitrogen with an Iron Porphyrin Complex

Cited by 12 publications

References 35 publications

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Exploring the Micropore Functional Mechanism of N₂O Adsorption by the Eucalyptus Bark-based Porous Carbon

Redox Behavior and Kinetics of Hydroxo Ligand Exchange on Iron Tetraphenylporphyrin: Comparison with Chloro Exchange and Consequences for Its Role in Self-Modulation of Molecular Catalysis of Electrochemical Reactions

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Selective Electrocatalytic Reduction of Nitrous Oxide to Dinitrogen with an Iron Porphyrin Complex

Cited by 12 publications

References 35 publications

High-Efficiency Electrocatalytic Reduction of N2O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

High-Efficiency Electrocatalytic Reduction of N2O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Exploring the Micropore Functional Mechanism of N2O Adsorption by the Eucalyptus Bark-based Porous Carbon

Redox Behavior and Kinetics of Hydroxo Ligand Exchange on Iron Tetraphenylporphyrin: Comparison with Chloro Exchange and Consequences for Its Role in Self-Modulation of Molecular Catalysis of Electrochemical Reactions

Contact Info

Product

Resources

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High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

High-Efficiency Electrocatalytic Reduction of N₂O with Single-Atom Cu Supported on Nitrogen-Doped Carbon

Exploring the Micropore Functional Mechanism of N₂O Adsorption by the Eucalyptus Bark-based Porous Carbon