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

Advanced Functional Materials, Год журнала: 2024, Номер 34(36)

Опубликована: Апрель 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.

Язык: Английский

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

Nano Energy, Год журнала: 2024, Номер 125, С. 109594 - 109594

Опубликована: Апрель 6, 2024

Язык: Английский

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

ACS Nano, Год журнала: 2024, Номер 18(20), С. 13141 - 13149

Опубликована: Май 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.

Язык: Английский

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Electrocatalytic nitrite reduction to ammonia on In1Cu single atom alloy

Chemical Engineering Journal, Год журнала: 2024, Номер 489, С. 151410 - 151410

Опубликована: Апрель 17, 2024

Язык: Английский

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Synergistic Cu Single Atoms and MoS₂‐Edges for Tandem Electrocatalytic Reduction of NO₃⁻ and CO₂ to Urea

Advanced Energy Materials, Год журнала: 2024, Номер 14(43)

Опубликована: Авг. 16, 2024

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) under ambient conditions is recognized as an appealing approach for effective sustainable urea production, while it requires high‐efficiency UENC electrocatalysts to promote the C─N coupling hydrogenation processes. Herein, single‐atom Cu anchored on MoS (Cu 1 ‐MoS ) explored a highly active selective catalyst. Theoretical calculations operando spectroscopic characterizations unveil synergistic tandem catalysis UENC, where single atoms trigger early coupling, ‐edges key step * NH COOHNH generation. Strikingly, equipped in flow cell achieves excellent performance with maximum urea‐Faradaic efficiency 57.02% at −0.6 V corresponding yield rate 23.3 mmol h −1 g , surpassing nearly all previously reported catalysts.

Язык: Английский

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Electrocatalysts with atomic-level site for nitrate reduction to ammonia

Journal of Energy Chemistry, Год журнала: 2024, Номер 96, С. 642 - 668

Опубликована: Май 27, 2024

Язык: 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, Год журнала: 2024, Номер 12(15), С. 5979 - 5990

Опубликована: Апрель 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.

Язык: Английский

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Strategic regulation of nitrogen-containing intermediates for enhanced nitrate reduction over Co3O4/SiC catalyst having multiple active centers

Journal of Energy Chemistry, Год журнала: 2024, Номер 96, С. 291 - 299

Опубликована: Май 10, 2024

Язык: 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, Год журнала: 2024, Номер 493, С. 152659 - 152659

Опубликована: Май 29, 2024

Язык: Английский

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

Fuel, Год журнала: 2024, Номер 369, С. 131750 - 131750

Опубликована: Апрель 22, 2024

Язык: Английский

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