Tandem electrocatalytic N2 fixation via proton-coupled electron transfer

Nature, Journal Year: 2022, Volume and Issue: 609(7925), P. 71 - 76

Published: Aug. 31, 2022

Language: Английский

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Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(1)

Published: April 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Language: Английский

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Coadsorption of NRR and HER Intermediates Determines the Performance of Ru-N₄ toward Electrocatalytic N₂ Reduction

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(4), P. 2505 - 2512

Published: Feb. 3, 2022

Electrochemical N2 reduction (NRR) to ammonia is seriously limited by the competing hydrogen evolution reaction (HER), but atomic-scale factors controlling HER/NRR competition are unknown. Herein we unveil mechanism, thermodynamics, and kinetics determining efficiency on state-of-the-art NRR electrocatalyst, Ru-N4, using grand canonical ensemble density functional theory (GCE-DFT). We show that NRR/HER intermediates coadsorb catalyst where suppress HER selectivity determined initial step forming *NNH or *H. Our results provide crucial insight into complex competition, necessity of GCE-DFT calculations, suggest ways improve selectivity.

Language: Английский

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Sulfur-deficient Bi2S3−x synergistically coupling Ti3C2Tx-MXene for boosting electrocatalytic N2 reduction

Nano Research, Journal Year: 2022, Volume and Issue: 15(5), P. 3991 - 3999

Published: Feb. 8, 2022

Language: Английский

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Microscopic-Level Insights into the Mechanism of Enhanced NH₃ Synthesis in Plasma-Enabled Cascade N₂ Oxidation–Electroreduction System

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(23), P. 10193 - 10200

Published: May 19, 2022

Integrated/cascade plasma-enabled N2 oxidation and electrocatalytic NOx– (where x = 2, 3) reduction reaction (pNOR-eNOx–RR) holds great promise for the renewable synthesis of ammonia (NH3). However, corresponding activated effects process plasma toward O2 molecules mechanism eNOx–RR to NH3 are unclear need be further uncovered, which largely limits large-scale deployment this integration technology. Herein, we systematically investigate activation recombination processes molecules, more meaningfully, at a microscopic level is also decoupled using copper (Cu) nanoparticles as representative electrocatalyst. The concentration produced NOx in pNOR system confirmed function length spark discharge well volumetric ratio feeding gas. successive protonation key N-containing intermediates (e.g., −NH2) detected with situ infrared spectroscopy. Besides, Raman spectroscopy reveals dynamic reconstruction Cu during process. nanoparticle-driven pNOR-eNOx–RR can finally achieve high yield rate ∼40 nmol s–1 cm–2 Faradaic efficiency nearly 90%, overperforming benchmarks reported literature. It anticipated that work will stimulate practical development green electrosynthesis directly from air water under ambient conditions.

Language: Английский

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Elucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 28, 2023

Electrocatalytic reduction of waste nitrates (NO3-) enables the synthesis ammonia (NH3) in a carbon neutral and decentralized manner. Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts demonstrate high catalytic activity uniquely favor mono-nitrogen products. However, reaction fundamentals remain largely underexplored. Herein, we report set 14; 3d-, 4d-, 5d- f-block M-N-C catalysts. The selectivity NO3- to NH3 media, with specific focus on deciphering role NO2- intermediate cascade, reveals strong correlations (R=0.9) between for NH3. Moreover, theoretical computations reveal associative/dissociative adsorption pathways evolution, over normal M-N4 sites their oxo-form (O-M-N4) oxyphilic metals. This work provides platform designing multi-element NO3RR cascades single-atom or hybridization extended surfaces.

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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Highly Durable and Selective Fe- and Mo-Based Atomically Dispersed Electrocatalysts for Nitrate Reduction to Ammonia via Distinct and Synergized NO₂^– Pathways

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(11), P. 6651 - 6662

Published: May 20, 2022

Aimed toward the pursuit of manufacturing ammonia in a carbon-neutral and decentralized manner, electrocatalytic nitrate reduction reaction (NO3RR) not only promises an effective route for synthesis but also offers potential advantages to wastewater remediation. Here, we describe efficacy bioinspired, atomically dispersed catalysts NO3RR aqueous media via catalytic cascade. Compared nanoparticles with extended surfaces, are largely underexplored this field, despite their intrinsic selectivity mono-nitrogen species over dinitrogen counterparts. Herein, specifically report on series nitrogen-coordinated mono- bimetallic, dispersed, iron- molybdenum-based electrocatalysts NO3RR. The key role *NO2/NO2– intermediates was identified both computationally experimentally, wherein Fe–N4 sites Mo–N4/*O–Mo–N4 carried distinct associative dissociative adsorption NO3– molecules, respectively. By integrating individual Fe Mo single bimetallic catalyst, unique pathways were synergized, achieving Faradaic efficiency 94% ammonia. Furthermore, robustness FeMo–N–C catalyst highlighted by five consecutive 12 h electrolysis cycles being maintained above 90% entire 60 h. utilization cascades, synergizing heterogeneous single-atom sites, is unconstrained linear scaling relations sheds light designing highly selective, efficient, durable synthesis.

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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