Tandem Electrocatalytic Reduction of Nitrite to Ammonia on Rhodium–Copper Single Atom Alloys

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: April 23, 2024

Abstract Electrocatalytic reduction of NO 2 − to NH 3 (NO RR) presents a fascinating approach for simultaneously migrating pollutants and producing valuable . In this study, single‐atom Rh‐alloyed copper (CuRh 1 ) is explored as highly active selective catalyst toward the RR. Combined theoretical calculations in situ FTIR/EPR spectroscopic experiments uncover synergistic effect Rh Cu promote RR energetics CuRh through tandem catalysis pathway, which activates preliminary adsorption hydrogenation → *NO *NOOH *NO), while generated on then transferred substrate promotes rate‐determining step *NHO synthesis. As result, equipped flow cell an unprecedented yield rate 2191.6 µmol h −1 cm −2 ‐Faradaic efficiency 98.9% at high current density 322.5 mA , well long‐term stability 100 electrolysis.

Language: Английский

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p-d hybridized In-Co dual sites promote nitrite electroreduction to ammonia at high current density

Nano Energy, Journal Year: 2024, Volume and Issue: 125, P. 109594 - 109594

Published: April 6, 2024

Language: Английский

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P-Block Antimony–Copper Single-Atom Alloys for Selective Nitrite Electroreduction to Ammonia

ACS Nano, Journal Year: 2024, Volume and Issue: 18(20), P. 13141 - 13149

Published: May 8, 2024

Electrocatalytic reduction of NO2– to NH3 (NO2RR) offers an effective method for alleviating pollution and generating valuable NH3. Herein, a p-block single-atom alloy, namely, isolated Sb alloyed in Cu substrate (Sb1Cu), is explored as durable high-current-density NO2RR catalyst. As revealed by the theoretical calculations operando spectroscopic measurements, we demonstrate that Sb1 incorporation can not only hamper competing hydrogen evolution reaction but also optimize d-band center Sb1Cu intermediate adsorption energies boost protonation energetics NO2–-to-NH3 conversion. Consequently, integrated flow cell achieves outstanding yield rate 2529.4 μmol h–1 cm–2 FENH3 95.9% at high current density 424.2 mA cm–2, well durability 100 h electrolysis.

Language: Английский

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Electrocatalytic nitrite reduction to ammonia on In1Cu single atom alloy

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 489, P. 151410 - 151410

Published: April 17, 2024

Language: Английский

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Electrocatalysts with atomic-level site for nitrate reduction to ammonia

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 96, P. 642 - 668

Published: May 27, 2024

Language: Английский

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Core–Shell Engineering Boosted Active Hydrogen Generation in Cu_2–xS/MoS₂ Quantum Dots for Efficient Electrocatalytic Nitrate Reduction to Ammonia

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(15), P. 5979 - 5990

Published: April 1, 2024

The electrochemical nitrate reduction reaction (NO3RR) emerges as a promising method for ammonia (NH3) production, which faces the dilemma of inhibiting hydrogen evolution (HER) and promoting active (Hads) supply hydrogenation nitrogen intermediates. Here, core–shell structure engineering strategy is developed Cu2–xS/MoS2, where strong Hads adsorption storage capacity can accelerate As result, an eminent NH3 yield 0.178 mmol h–1 cm–2 Faradaic efficiency 84.5% were achieved. A series tests demonstrate that tuning Cu2–xS/MoS2 interface improve activity conversion NO2–, while avoiding HER effectively retain Hads. density functional theory calculation further demonstrates has *H retention ability to promote NO3RR process. This work offers novel perspective on manipulation generation NO3RR.

Language: Английский

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Electrocatalytic nitrogen reduction to ammonia at low overpotentials based on tungsten carbide doped by non-precious metal single cobalt atoms

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 493, P. 152659 - 152659

Published: May 29, 2024

Language: Английский

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NH₃ Synthesis via Electrocatalytic N₂ Reduction Reaction on the Defective Surfaces of Nb₂Mo₂C₃T_x MXenes: Theoretical and Experimental Studies

Energy & Fuels, Journal Year: 2024, Volume and Issue: 38(13), P. 11815 - 11823

Published: June 12, 2024

Electrocatalytic N2 reduction reaction (NRR) is a low-cost and environmental friendly strategy for NH3 synthesis but yet needs more fundamental applied research. Herein, we explored the NRR activity of bimetal Nb2Mo2C3Tx MXene catalyst via both theoretical experimental studies. Density functional theory calculations revealed that horizontal adsorption can be most stable mode molecule, alternating mechanism showed downhill free energy input all through reaction. More importantly, surface Nb Mo terminations MXenes facilitate demonstrate comparable to benchmark Ru. In experiment, achieved an yield 20.77 μg h–1 mgcat–1 high Faraday efficiency 31.0%, demonstrating excellent selectivity durability. Internal carbon layers ensured fast electron transfer avoided self-aggregation active sites. Structural defects also played important role in its because formation vast unsaturated Nb/Mo atoms.

Language: Английский

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Emerging Advances in Cu-based electrocatalysts for electrochemical nitrate reduction (NO3RR)

Surfaces and Interfaces, Journal Year: 2024, Volume and Issue: 48, P. 104294 - 104294

Published: April 16, 2024

Language: Английский

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Tuning electronic environment of B sites in boron carbonitride nanoribbon boosts catalytic activity of reducing N2 to NH3

Fuel, Journal Year: 2024, Volume and Issue: 369, P. 131750 - 131750

Published: April 22, 2024

Language: Английский

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