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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Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings

Nature Energy, Год журнала: 2021, Номер 6(11), С. 1026 - 1034

Опубликована: Окт. 28, 2021

Язык: Английский

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Can sustainable ammonia synthesis pathways compete with fossil-fuel based Haber–Bosch processes?

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2535 - 2548

Опубликована: Янв. 1, 2021

This analysis presents system level of three stages along the transition towards sustainable synthesis ammonia.

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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Main-group elements boost electrochemical nitrogen fixation

Chem, Год журнала: 2021, Номер 7(12), С. 3232 - 3255

Опубликована: Ноя. 9, 2021

Язык: Английский

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Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 49 - 113

Опубликована: Ноя. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Язык: Английский

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High-Efficiency N₂ Electroreduction Enabled by Se-Vacancy-Rich WSe_2–x in Water-in-Salt Electrolytes

ACS Nano, Год журнала: 2022, Номер 16(5), С. 7915 - 7925

Опубликована: Апрель 22, 2022

Electrocatalytic nitrogen reduction reaction (NRR) is a promising approach for renewable NH3 production, while developing the NRR electrocatalysis systems with both high activity and selectivity remains significant challenge. Herein, we combine catalyst electrolyte engineering to achieve high-efficiency enabled by Se-vacancy-rich WSe2-x in water-in-salt (WISE). Extensive characterizations, theoretical calculations, situ X-ray photoelectron/Raman spectroscopy reveal that WISE ensures suppressed H2 evolution, improved N2 affinity on surface, as well an enhanced π-back-donation ability of active sites, thereby promoting NRR. As result, excellent faradaic efficiency 62.5% yield 181.3 μg h-1 mg-1 achieved 12 m LiClO4, which among highest performances reported date.

Язык: Английский

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Isolating Single and Few Atoms for Enhanced Catalysis

Advanced Materials, Год журнала: 2022, Номер 34(39)

Опубликована: Май 17, 2022

Abstract Atomically dispersed metal catalysts have triggered great interest in the field of catalysis owing to their unique features. Isolated single or few atoms can be anchored on substrates via chemical bonding space confinement maximize atom utilization efficiency. The key challenge lies precisely regulating geometric and electronic structure active centers, thus significantly influencing catalytic properties. Although several reviews been published preparation, characterization, application single‐atom (SACs), comprehensive understanding SACs, dual‐atom (DACs), atomic clusters has never systematically summarized. Here, recent advances engineering local environments state‐of‐the‐art DACs, for enhanced performance are highlighted. Firstly, various synthesis approaches presented. Then, special attention is focused elucidation terms state coordination structure. Furthermore, a summary isolated applications thermocatalysis, electrocatalysis, photocatalysis provided. Finally, potential challenges future opportunities this emerging This review will pave way regulate microenvironment site boosting processes.

Язык: Английский

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Metal–organic framework supported Au nanoparticles with organosilicone coating for high-efficiency electrocatalytic N2 reduction to NH3

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 302, С. 120840 - 120840

Опубликована: Окт. 25, 2021

Язык: Английский

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Local Spin‐State Tuning of Iron Single‐Atom Electrocatalyst by S‐Coordinated Doping for Kinetics‐Boosted Ammonia Synthesis

Advanced Materials, Год журнала: 2022, Номер 34(28)

Опубликована: Май 6, 2022

The electrochemical nitrogen reduction reaction (e-NRR) is envisaged as alternative technique to the Haber-Bosch process for NH3 synthesis. However, how develop highly active e-NRR catalysts faces daunting challenges. Herein, a viable strategy manipulate local spin state of isolated iron sites through S-coordinated doping (FeSA -NSC) reported. Incorporation S in coordination FeSA -NSC can induce transition spin-polarization configuration with formation medium-spin-state Fe (t2g 6 eg 1), which beneficial facilitating electrons penetrate antibonding π-orbital nitrogen. As consequence, record-high current density up 10 mA cm-2 be achieved, together high selectivity ≈10% flow cell reactor. Both experimental and theoretical analyses indicate that monovalent Fe(I) atomic center after accelerates N2 activation protonation rate-determining step *N2 *NNH.

Язык: Английский

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