Urea Electrosynthesis from Nitrate and CO₂ on Diatomic Alloys

Advanced Materials, Год журнала: 2024, Номер 36(30)

Опубликована: Июнь 14, 2024

Abstract Urea electrosynthesis from co–electrolysis of NO 3 − and CO 2 (UENC) offers a promising technology for achieving sustainable efficient urea production. Herein, diatomic alloy catalyst (CuPd 1 Rh –DAA), with mutually isolated Pd atoms alloyed on Cu substrate, is theoretically designed experimentally confirmed to be highly active selective UENC catalyst. Combining theoretical computations operando spectroscopic characterizations reveals the synergistic effect –Cu sites promote via tandem catalysis mechanism, where site triggers early C–N coupling promotes *CO –to–*CO NH steps, while facilitates subsequent protonation step *COOHNH toward formation. Impressively, CuPd –DAA assembled in flow cell presents highest Faradaic efficiency 72.1% yield rate 53.2 mmol h −1 g cat at −0.5 V versus RHE, representing nearly performance among all reported catalysts.

Язык: Английский

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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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Electrochemical Nitrate Reduction to Ammonia on CuCo Nanowires at Practical Level

Advanced Functional Materials, Год журнала: 2024, Номер 34(44)

Опубликована: Май 27, 2024

Abstract Electrochemical reduction of nitrate (NO 3 RR) holds great promise for environmentally friendly ammonia production. Tandem catalysis is a promising strategy boosting the NO RR and inhibiting side effects, but it still challenged by lacking well‐designed catalysts to drive this catalytic process. Herein, study develops CuCo branched nanowires (CuCo NW) catalyst, which efficiently converts − NH on Co (111) Cu crystal facets through tandem mechanism. The in situ grown NW foam demonstrates remarkable Faraday efficiency 90.3% at 1.0 A cm −2 maintains stable operation 200 h 100 mA flow reactor. Density functional theory calculations suggest that initial absorption subsequent deoxygenation *NO leading formation 2 , followed its transfer further conversion *NH establish an optimal pathway managing rate‐determining steps individual surfaces RR. To showcase practical application scaling‐up prototype reactor continuous production, realizing gram‐level yield rate 1474.09 mg −1 91.26% practical‐level 20.0 A.

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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“Capture-activation-recapture” mechanism-guided design of double-atom catalysts for electrocatalytic nitrogen reduction

Journal of Energy Chemistry, Год журнала: 2024, Номер 96, С. 437 - 447

Опубликована: Май 15, 2024

Язык: Английский

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Advancements in Electrocatalytic Nitrogen Reduction: A Comprehensive Review of Single‐Atom Catalysts for Sustainable Ammonia Synthesis

Small, Год журнала: 2024, Номер 20(32)

Опубликована: Март 22, 2024

Abstract Electrocatalytic nitrogen reduction technology seamlessly aligns with the principles of environmentally friendly chemical production. In this paper, a comprehensive review recent advancements in electrocatalytic NH 3 synthesis utilizing single‐atom catalysts (SACs) is offered. Into research and applications three categories SACs: noble metals (Ru, Au, Rh, Ag), transition (Fe, Mo, Cr, Co, Sn, Y, Nb), nonmetallic (B) context ammonia delved. In‐depth insights into material preparation methods, coordination patterns, characteristics reaction (NRR) are provided. The systematic comparison capabilities various SAC types offers framework for their integration NRR. Additionally, challenges, potential solutions, future prospects incorporating SACs endeavors discussed.

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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Phosphorus-doped Ti₃C₂T_x MXene nanosheets enabling ambient NH₃ synthesis with high current densities

Chemical Communications, Год журнала: 2024, Номер 60(66), С. 8728 - 8731

Опубликована: Янв. 1, 2024

Herein, we show that P-doped Ti

Язык: Английский

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CoNiOOH nanosheets array enables highly effective value-added chemicals production via nitrite and sulfide electrolysis

Chemical Engineering Journal, Год журнала: 2024, Номер unknown, С. 155799 - 155799

Опубликована: Сен. 1, 2024

Язык: Английский

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