Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120010 - e9120010

Опубликована: Май 30, 2022

To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals minimal carbon emissions. The background of such N-cycles, as fixation, ammonia oxidation, nitrate reduction, is briefly introduced here. discussion emerging nanostructures in various conversion reactions focused on architecture/compositional design, electrochemical performances, reaction mechanisms, instructive tests. Energy device advancements for achieving more functions well in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed less discussed C–N coupling summarized. We classify inorganic sources that each other under an applied voltage into three types, namely, abundant nitrogen, toxic (nitrite), oxides, useful compounds ammonia, hydrazine, hydroxylamine, goal providing critical insights strategies facilitate development our circular economy.

Язык: Английский

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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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Single‐Atom Bi Alloyed Pd Metallene for Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Год журнала: 2023, Номер 33(12)

Опубликована: Янв. 15, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) holds a great promise for attaining both NH electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi 1 Pd) is reported as highly effective NO RR catalyst, showing near 100% ‐Faradaic efficiency with the corresponding yield 33.8 mg h −1 cm −2 at −0.6 V versus RHE, surpassing those almost all ever catalysts. In‐depth theoretical operando spectroscopic investigations unveil that electronically couples its neighboring atoms synergistically activate − destabilize *NO on Pd, leading reduced energy barrier potential‐determining step (*NO→*NOH) enhanced protonation energetics ‐to‐NH pathway.

Язык: Английский

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Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

ACS Nano, Год журнала: 2023, Номер 17(2), С. 1081 - 1090

Опубликована: Янв. 11, 2023

The electrochemical nitrate reduction to ammonia reaction (NO3RR) has emerged as an appealing route for achieving both wastewater treatment and production. Herein, sub-nm RuOx clusters anchored on a Pd metallene (RuOx/Pd) are reported highly effective NO3RR catalyst, delivering maximum NH3-Faradaic efficiency of 98.6% with corresponding NH3 yield rate 23.5 mg h–1 cm–2 partial current density 296.3 mA at −0.5 V vs RHE. Operando spectroscopic characterizations combined theoretical computations unveil the synergy enhance energetics through mechanism hydrogen spillover hydrogen-bond interactions. In detail, activates NO3– form intermediates, while dissociates H2O generate *H, which spontaneously migrates RuOx/Pd interface via process. Further interactions between spillovered *H intermediates makes desorb from participate in intermediate hydrogenation, contributing enhanced activity NO3–-to-NH3 conversion.

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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Recent progress in electrocatalytic nitrogen reduction to ammonia (NRR)

Coordination Chemistry Reviews, Год журнала: 2022, Номер 478, С. 214981 - 214981

Опубликована: Дек. 25, 2022

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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Vacancy Defects in 2D Transition Metal Dichalcogenide Electrocatalysts: From Aggregated to Atomic Configuration

Advanced Materials, Год журнала: 2022, Номер 35(50)

Опубликована: Окт. 3, 2022

Abstract Vacancy defect engineering has been well leveraged to flexibly shape comprehensive physicochemical properties of diverse catalysts. In particular, growing research effort devoted chalcogen anionic vacancies (S/Se/Te) 2D transition metal dichalcogenides (2D TMDs) toward the ultimate performance limit electrocatalytic hydrogen evolution reaction (HER). spite remarkable progress achieved in past decade, systematic and in‐depth insights into state‐of‐the‐art vacancy for 2D‐TMDs‐based electrocatalysis are still lacking. Herein, this review delivers a full picture evolving from aggregated atomic configurations covering their development background, controllable manufacturing, thorough characterization, representative HER application. Of particular interest, deep‐seated correlations between specific regulation routes resulting catalytic improvement logically clarified terms rearrangement, charge redistribution, energy band variation, intermediate adsorption–desorption optimization, charge/mass transfer facilitation. Beyond that, broader vision is cast cutting‐edge fields vacancy‐engineering‐based single‐atom catalysis dynamic structure–performance across catalyst service lifetime. Together with critical discussion on residual challenges future prospects, sheds new light rational design advanced catalysts navigates application high‐efficiency conversion storage fields.

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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Ultra-efficient N2 electroreduction achieved over a rhodium single-atom catalyst (Rh1/MnO2) in water-in-salt electrolyte

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 316, С. 121651 - 121651

Опубликована: Июнь 21, 2022

Язык: Английский

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