Direct Eight-Electron N₂O Electroreduction to NH₃ Enabled by an Fe Double-Atom Catalyst

Nano Letters, Journal Year: 2024, Volume and Issue: 24(28), P. 8502 - 8509

Published: July 1, 2024

N2O is a dominant atmosphere pollutant, causing ozone depletion and global warming. Currently, electrochemical reduction of has gained increasing attention to remove N2O, but its product worthless N2. Here, we propose direct eight-electron (8e) pathway electrochemically convert into NH3. As proof concept, using density functional theory calculation, an Fe2 double-atom catalyst (DAC) anchored by N-doped porous graphene (Fe2@NG) was screened out be the most active selective for electroreduction toward NH3 via novel 8e pathway, which benefits from unique bent adsorption configuration. Guided theoretical prediction, Fe2@NG DAC fabricated experimentally, it can achieve high N2O-to-NH3 Faradaic efficiency 77.8% with large yield rate 2.9 mg h–1 cm–2 at −0.6 V vs RHE in neutral electrolyte. Our study offers feasible strategy synthesize pollutant simultaneous removal.

Language: Английский

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Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Jan. 27, 2024

Li-CO2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction inert CO2 often results in formation Li2CO3, causing dip output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to cathode via Cu(II) coordination compound benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents shuttle effect sluggish kinetics associated with soluble mediators. Results show that electrochemically reduced Cu(I) mediator efficiently captures CO2, facilitating Li2C2O4 through dimerization reaction involving dimeric oxalate intermediate. The battery employing boasts higher discharge 2.8 V, lower charge potential 3.7 superior cycling performance over 400 cycles. Simultaneously, successful development pouch propels metal-CO2 closer practical application.

Language: Английский

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Progress and challenges in nitrous oxide decomposition and valorization

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(16), P. 8379 - 8423

Published: Jan. 1, 2024

Nitrous oxide (N

Language: Английский

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Bimetallic NiCu catalyst derived from spent MOF adsorbent for efficient photocatalytic CO2 reduction

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 497, P. 154701 - 154701

Published: Aug. 10, 2024

Language: Английский

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Nitrogen oxyanion deoxygenation: Redox chemistry and oxygen atom transfer reactions

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 530, P. 216490 - 216490

Published: Feb. 3, 2025

Language: Английский

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A family of first-row metal complexes bound by a new pentadentate ligand

Journal of Coordination Chemistry, Journal Year: 2025, Volume and Issue: unknown, P. 1 - 15

Published: May 21, 2025

Language: Английский

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Open-Cage Copper Complexes Modulate Coordination and Charge Transfer

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(26), P. 12081 - 12088

Published: June 19, 2024

This study presents a novel copper-based redox shuttle that employs the PY5 pentadentate polypyridyl ligand in dye-sensitized solar cell (DSSC). The [Cu(PY5)]

Language: Английский

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Bioinspired copper-catalysed nitrous oxide reduction with simultaneous N–H or O–H bond oxidation

Catalysis Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Tuning selectivities with oxidants: O 2 oxidises methanol to the carboxylate level and N it formaldehyde level.

Language: Английский

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Deoxygenation reactions of nitrous oxide assisted by oriented external electric field

International Journal of Quantum Chemistry, Journal Year: 2024, Volume and Issue: 124(9)

Published: April 27, 2024

Abstract Due largely to the high stability and potential ozone‐depleting, transformation of greenhouse gas nitrous oxide has gained much attentions. In present paper, a new insight into deoxygenation with silane was reported by using oriented external electric field (OEEF) as catalytic strategy. When OEEF employed, reaction barrier marvelously decreased it along positive NO/OSi bond‐axis. Especially strength is 300 × 10 −4 a.u., differences are up 22.4/18.3 kcal mol −1 compared that nonfield. addition, once H atom in SiH 4 replaced methyl, two modes were obtained, which process easier when N 2 O captured attached Si atom, not C atom. Further, solvent effects also considered, but weak influence obtained.

Language: Английский

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Copper(I) Catalysed Diboron(4) Reduction of Nitrous Oxide

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(45)

Published: July 16, 2024

Abstract A process for the catalytic reduction of nitrous oxide using NHC‐ligated copper(I) tert ‐butoxide precatalysts and B 2 pin as reductant is reported. These reactions proceed under mild conditions via copper(I)‐boryl intermediates which react with N O by facile O‐atom insertion into Cu−B bond liberate . Turnover numbers >800 can be achieved at 80 °C 1 bar O.

Language: Английский

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