Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

ACS Nano, Journal Year: 2023, Volume and Issue: 17(2), P. 1081 - 1090

Published: Jan. 11, 2023

The electrochemical nitrate reduction to ammonia reaction (NO3RR) has emerged as an appealing route for achieving both wastewater treatment and production. Herein, sub-nm RuOx clusters anchored on a Pd metallene (RuOx/Pd) are reported highly effective NO3RR catalyst, delivering maximum NH3-Faradaic efficiency of 98.6% with corresponding NH3 yield rate 23.5 mg h–1 cm–2 partial current density 296.3 mA at −0.5 V vs RHE. Operando spectroscopic characterizations combined theoretical computations unveil the synergy enhance energetics through mechanism hydrogen spillover hydrogen-bond interactions. In detail, activates NO3– form intermediates, while dissociates H2O generate *H, which spontaneously migrates RuOx/Pd interface via process. Further interactions between spillovered *H intermediates makes desorb from participate in intermediate hydrogenation, contributing enhanced activity NO3–-to-NH3 conversion.

Language: Английский

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Single‐Atom Bi Alloyed Pd Metallene for Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(12)

Published: Jan. 15, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) holds a great promise for attaining both NH electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi 1 Pd) is reported as highly effective NO RR catalyst, showing near 100% ‐Faradaic efficiency with the corresponding yield 33.8 mg h −1 cm −2 at −0.6 V versus RHE, surpassing those almost all ever catalysts. In‐depth theoretical operando spectroscopic investigations unveil that electronically couples its neighboring atoms synergistically activate − destabilize *NO on Pd, leading reduced energy barrier potential‐determining step (*NO→*NOH) enhanced protonation energetics ‐to‐NH pathway.

Language: Английский

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High-Efficiency N₂ Electroreduction Enabled by Se-Vacancy-Rich WSe_2–x in Water-in-Salt Electrolytes

ACS Nano, Journal Year: 2022, Volume and Issue: 16(5), P. 7915 - 7925

Published: April 22, 2022

Electrocatalytic nitrogen reduction reaction (NRR) is a promising approach for renewable NH3 production, while developing the NRR electrocatalysis systems with both high activity and selectivity remains significant challenge. Herein, we combine catalyst electrolyte engineering to achieve high-efficiency enabled by Se-vacancy-rich WSe2-x in water-in-salt (WISE). Extensive characterizations, theoretical calculations, situ X-ray photoelectron/Raman spectroscopy reveal that WISE ensures suppressed H2 evolution, improved N2 affinity on surface, as well an enhanced π-back-donation ability of active sites, thereby promoting NRR. As result, excellent faradaic efficiency 62.5% yield 181.3 μg h-1 mg-1 achieved 12 m LiClO4, which among highest performances reported date.

Language: Английский

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Lewis Acid Fe‐V Pairs Promote Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(13)

Published: Jan. 18, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) has been recognized as an appealing approach realize both sustainable NH production and waste removal. Herein, from the perspective Lewis acid‐base interaction, a single‐atom Fe‐doped V 2 O 5 (Fe‐V ) catalyst enriched is designed with acid sites, which present maximum ‐Faradaic efficiency 97.1% corresponding yield 12.5 mg h −1 cm −2 at –0.7 versus RHE. Mechanistic studies based on theoretical calculations operando spectroscopic characterizations identify creation Fe‐V pairs , can synergetically activate NO − promote hydrogenation energetics, restrain hydrogen evolution, leading enhanced RR activity selectivity.

Language: Английский

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Recent progress in electrocatalytic nitrogen reduction to ammonia (NRR)

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 478, P. 214981 - 214981

Published: Dec. 25, 2022

Language: Английский

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Iridium single-atom catalyst for highly efficient NO electroreduction to NH3

Nano Research, Journal Year: 2023, Volume and Issue: 16(7), P. 8737 - 8742

Published: March 8, 2023

Language: Английский

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Amorphization engineered VSe_2−x nanosheets with abundant Se-vacancies for enhanced N₂ electroreduction

Journal of Materials Chemistry A, Journal Year: 2021, Volume and Issue: 10(4), P. 1742 - 1749

Published: Dec. 24, 2021

Amorphous VSe 2− x nanosheets with abundant Se-vacancies (V Se ) showed dramatically enhanced NRR activity and selectivity, attributed to the amorphization-triggered that promote impeding H 2 evolution.

Language: Английский

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Ultra-efficient N2 electroreduction achieved over a rhodium single-atom catalyst (Rh1/MnO2) in water-in-salt electrolyte

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 316, P. 121651 - 121651

Published: June 21, 2022

Language: Английский

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B-doped MoS2 for nitrate electroreduction to ammonia

Journal of Colloid and Interface Science, Journal Year: 2022, Volume and Issue: 629, P. 950 - 957

Published: Sept. 13, 2022

Language: Английский

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Atomically Fe-doped MoS2−x with Fe-Mo dual sites for efficient electrocatalytic NO reduction to NH3

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 324, P. 122241 - 122241

Published: Nov. 29, 2022

Language: Английский

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