Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 3, 2023

We demonstrate the great feasibility of MBenes as a new class tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As proof concept, FeB2 is first employed model MBene catalyst NO3 RR, showing maximum NH3 -Faradaic efficiency 96.8 % with corresponding yield 25.5 mg h-1 cm-2 at -0.6 V vs. RHE. Mechanistic studies reveal that exceptional RR activity arises from catalysis mechanism, is, B sites activate NO3- form intermediates, while Fe dissociate H2 O and increase *H supply on promote intermediate hydrogenation enhance -to-NH3 conversion.

Язык: Английский

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Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction

Chem, Год журнала: 2023, Номер 9(7), С. 1768 - 1827

Опубликована: Июнь 21, 2023

Язык: Английский

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Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Июнь 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Язык: Английский

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Unveiling Cutting‐Edge Developments in Electrocatalytic Nitrate‐to‐Ammonia Conversion

Advanced Materials, Год журнала: 2024, Номер 36(16)

Опубликована: Янв. 11, 2024

The excessive enrichment of nitrate in the environment can be converted into ammonia (NH

Язык: Английский

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Lewis Acid Fe‐V Pairs Promote Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Год журнала: 2023, Номер 33(13)

Опубликована: Янв. 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.

Язык: Английский

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

Nano Research, Год журнала: 2023, Номер 16(7), С. 8737 - 8742

Опубликована: Март 8, 2023

Язык: Английский

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p-Block Antimony Single-Atom Catalysts for Nitric Oxide Electroreduction to Ammonia

ACS Energy Letters, Год журнала: 2023, Номер 8(3), С. 1281 - 1288

Опубликована: Фев. 3, 2023

Electrocatalytic NO reduction to NH3 (NORR) offers a prospective approach attain both harmful removal and efficient electrosynthesis. Main-group p-block metals are promising NORR candidates but still lack adequate exploration. Herein, Sb single atoms confined in amorphous MoO3 (Sb1/a-MoO3) designed as an catalyst, exhibiting the highest yield rate of 273.5 μmol h–1 cm–2 NO-to-NH3 Faradaic efficiency 91.7% at −0.6 V vs RHE. In situ spectroscopic characterizations theoretical computations reason that outstanding performance Sb1/a-MoO3 arises from isolated Sb1 sites, which can optimize adsorption *NO/*NHO lower reaction energy barriers simultaneously exhibit higher affinity than H2O/H species. Moreover, our strategy be extended prepare Bi1/a-MoO3, showing high property, demonstrating immense potential metal single-atom catalysts toward high-performing electrocatalysis.

Язык: Английский

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Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study

Journal of the American Chemical Society, Год журнала: 2023, Номер 146(1), С. 668 - 676

Опубликована: Дек. 28, 2023

Electrochemical synthesis of ammonia via the nitrate reduction reaction (NO3RR) has been intensively researched as an alternative to traditional Haber–Bosch process. Most research focuses on low concentration range representative level in wastewater, leaving high range, which exists nuclear and fertilizer wastes, unexplored. The use a concentrated electrolyte (≥1 M) for higher rate production is hampered by poor hydrogen transfer kinetics. Herein, we demonstrate that cocatalytic system Ru/Cu2O catalyst enables NO3RR at 10.0 A 1 M 16 cm2 flow electrolyzer, with 100% faradaic efficiency toward ammonia. Detailed mechanistic studies deuterium labeling operando Fourier transform infrared (FTIR) spectroscopy allow us probe intermediate species Ru/Cu2O. Ab initio molecular dynamics (AIMD) simulations reveal adsorbed hydroxide Ru nanoparticles increases density hydrogen-bonded water network near Cu2O surface, promotes rate. Our work highlights importance engineering synergistic interactions cocatalysts addressing kinetic bottleneck electrosynthesis.

Язык: Английский

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Self-Tandem Electrocatalytic NO Reduction to NH₃ on a W Single-Atom Catalyst

Nano Letters, Год журнала: 2023, Номер 23(5), С. 1735 - 1742

Опубликована: Фев. 14, 2023

We design single-atom W confined in MoO3-x amorphous nanosheets (W1/MoO3-x) comprising W1-O5 motifs as a highly active and durable NORR catalyst. Theoretical operando spectroscopic investigations reveal the dual functions of to (1) facilitate activation protonation NO molecules (2) promote H2O dissociation while suppressing *H dimerization increase proton supply, eventually resulting self-tandem mechanism W1/MoO3-x greatly accelerate energetics NO-to-NH3 pathway. As result, exhibits highest NH3-Faradaic efficiency 91.2% NH3 yield rate 308.6 μmol h-1 cm-2, surpassing that most previously reported catalysts.

Язык: Английский

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Carbon‐Anchored Molybdenum Oxide Nanoclusters as Efficient Catalysts for the Electrosynthesis of Ammonia and Urea

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(19)

Опубликована: Март 13, 2023

Abstract The electrochemical NO 3 − reduction and its coupling with CO 2 can provide novel clean routes to synthesize NH urea, respectively. However, their practical application is still impeded by the lack of efficient catalysts desirable Faradaic efficiency (FE) yield rate. Herein, we report synthesis molybdenum oxide nanoclusters anchored on carbon black (MoO x /C) as electrocatalyst. It affords an outstanding FE 98.14 % rate 91.63 mg h −1 cat. in reduction. Besides, highest 27.7 a maximum urea 1431.5 μg toward also achieved. formation electron‐rich MoO highly unsaturated metal sites /C heterostructure beneficial for enhanced catalytic performance. Studies mechanism reveal that stabilization *NO *CO NOOH intermediates are critical synthesis,

Язык: Английский

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