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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Oxygen Vacancy-Mediated Selective C–N Coupling toward Electrocatalytic Urea Synthesis

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(26), С. 11530 - 11535

Опубликована: Июнь 24, 2022

The electrocatalytic C-N coupling for one-step urea synthesis under ambient conditions serves as the promising alternative to traditional synthetic protocol. However, hydrogenation of intermediate species hinders efficient synthesis. Herein, oxygen vacancy-enriched CeO2 was demonstrated electrocatalyst with stabilization crucial *NO via inserting into vacant sites, which is conducive subsequent process rather than protonation, whereas poor selectivity protonation observed on vacancy-deficient catalyst. vacancy-mediated selective distinguished and validated by in situ sum frequency generation spectroscopy. introduction vacancies tailors common catalyst carrier an a high yield rate 943.6 mg h-1 g-1, superior that partial noble-metal-based electrocatalysts. This work provides novel insights design developments systems.

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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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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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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Dynamic Reconstitution Between Copper Single Atoms and Clusters for Electrocatalytic Urea Synthesis

Advanced Materials, Год журнала: 2023, Номер 35(18)

Опубликована: Фев. 6, 2023

Electrocatalytic CN coupling between carbon dioxide and nitrate has emerged to meet the comprehensive demands of footprint closing, valorization waste, sustainable manufacture urea. However, identification catalytic active sites design efficient electrocatalysts remain a challenge. Herein, synthesis urea catalyzed by copper single atoms decorated on CeO2 support (denoted as Cu1 -CeO2 ) is reported. The catalyst exhibits an average yield rate 52.84 mmol h-1 gcat.-1 at -1.6 V versus reversible hydrogen electrode. Operando X-ray absorption spectra demonstrate reconstitution (Cu1 clusters (Cu4 during electrolysis. These electrochemically reconstituted Cu4 are real for electrocatalytic synthesis. Favorable reactions formation validated using operando synchrotron-radiation Fourier transform infrared spectroscopy theoretical calculations. Dynamic transformations single-atom configurations occur when applied potential switched open-circuit potential, endowing with superior structural electrochemical stabilities.

Язык: Английский

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Defect engineering of two-dimensional materials for advanced energy conversion and storage

Chemical Society Reviews, Год журнала: 2023, Номер 52(5), С. 1723 - 1772

Опубликована: Янв. 1, 2023

Defective two-dimensional (2D) materials show huge potential for energy-related fields. This review overviews the formation/evolution mechanisms and engineering strategies of defects in 2D materials, which enable enhanced electrode reaction kinetics.

Язык: Английский

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Regulating active hydrogen adsorbed on grain boundary defects of nano-nickel for boosting ammonia electrosynthesis from nitrate

Energy & Environmental Science, Год журнала: 2023, Номер 16(6), С. 2611 - 2620

Опубликована: Янв. 1, 2023

The grain boundary defect engineered Ni nanoparticles has been explored for boosting selective nitrate electroreduction to ammonia, and its NH 3 generation rate is much higher than those of the reported copper or noble metal-based catalysts.

Язык: Английский

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Recent advances in electrocatalytic ammonia synthesis

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2023, Номер 50, С. 6 - 44

Опубликована: Июль 1, 2023

Язык: Английский

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