Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: June 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

Language: Английский

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

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 11, 2024

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

Language: Английский

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Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(43)

Published: June 25, 2023

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading various environmental issues. To achieve green ammonia is a great challenge that extensively pursued recently. In review, most promising strategy, electrochemical nitrate reduction reaction (e‐NO 3 RR) for purpose comprehensively investigated give full understanding mechanism provide guidance future directions. Particularly, electrocatalysts focused realize high yield rate Faraday efficiency applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom metal‐free are systematically discussed review effects factors on catalytic performance in e‐NO RR. Accordingly, strategies, defects engineering, coordination environment modulating, surface controlling, hybridization, carefully improve performance, such intrinsic activity selectivity. Finally, perspectives challenges given out. This shall insightful advanced systems efficiently industry.

Language: Английский

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Recent progress and strategies on the design of catalysts for electrochemical ammonia synthesis from nitrate reduction

Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 10(12), P. 3489 - 3514

Published: Jan. 1, 2023

Ammonia (NH3) is an essential raw material in the production of fertilizers and a promising carbon-free energy carrier, however, its synthesis still depends on energy- capital-intensive Haber–Bosch process. Recently, electrochemical N2 reduction reaction has attracted significant interest as emerging method for NH3 under ambient conditions. However, limited solubility aqueous electrolyte strong NN bonds result low yield rate, inferior faradaic efficiency unsatisfactory selectivity, impeding further practical application. Considering high water nitrate (NO3−), NO3− (NO3−RR) become fascinating route achieving sustainable NH3, enormous progress been made this field. As consequence, review discusses mechanism systematically summarizes recent development electrocatalysts NO3−RR, including noble-metal-based materials, single-atom metal catalysts, transition-metal-based catalysts. Diverse design strategies catalysts to boost NO3−RR performance, such defect engineering, rational structure design, strain engineering constructing heterostructures, are discussed. This followed by illustration how robust understanding optimization affords fundamental insights into efficiency, selectivity electrocatalysts. Finally, we conclude with future perspectives critical issues, challenges research directions high-efficiency selective NH3.

Language: Английский

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Durable Electrocatalytic Reduction of Nitrate to Ammonia over Defective Pseudobrookite Fe₂TiO₅Nanofibers with Abundant Oxygen Vacancies

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(5)

Published: Dec. 5, 2022

We propose the pseudobrookite Fe2 TiO5 nanofiber with abundant oxygen vacancies as a new electrocatalyst to ambiently reduce nitrate ammonia. Such catalyst achieves large NH3 yield of 0.73 mmol h-1 mg-1cat. and high Faradaic Efficiency (FE) 87.6 % in phosphate buffer saline solution 0.1 M NaNO3 , which is lifted 1.36 96.06 at -0.9 V vs. RHE for nitrite conversion ammonia NaNO2 . It also shows excellent electrochemical durability structural stability. Theoretical calculation reveals enhanced conductivity this an extremely low free energy -0.28 eV adsorption presence vacant oxygen.

Language: Английский

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Weakened d–p orbital hybridization inin situreconstructed Ru/β-Co(OH)₂heterointerfaces for accelerated ammonia electrosynthesis from nitrates

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(6), P. 2483 - 2493

Published: Jan. 1, 2023

Electron-deficient Ru sites at Ru/Co(OH) 2 heterointerfaces weaken the d–p orbital hybridization ability and further facilitate desorption of ammonia intermediates, thereby achieving ultrahigh nitrate electroreduction activity towards ammonia.

Language: Английский

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Thermally Enhanced Relay Electrocatalysis of Nitrate-to-Ammonia Reduction over Single-Atom-Alloy Oxides

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(11), P. 7779 - 7790

Published: March 11, 2024

The electrochemical nitrate reduction reaction (NO3RR) holds promise for converting nitrogenous pollutants to valuable ammonia products. However, conventional electrocatalysis faces challenges in effectively driving the complex eight-electron and nine-proton transfer process of NO3RR while also competing with hydrogen evolution reaction. In this study, we present thermally enhanced nitrate-to-ammonia conversion over nickel-modified copper oxide single-atom alloy nanowires. catalyst demonstrates improved production performance a Faradaic efficiency approximately 80% yield rate 9.7 mg h–1 cm–2 at +0.1 V versus reversible electrode elevated cell temperatures. addition, system displays impressive stability, interference resistance, favorable energy consumption greenhouse gas emissions simulated industrial wastewater treatment. Complementary situ analyses confirm that significantly superior relay active species formed Ni sites facilitates thermal-field-coupled Cu surface-adsorbed *NOx hydrogenation. Theoretical calculations further support thermodynamic kinetic feasibility catalysis mechanism Ni1Cu model catalyst. This study introduces conceptual thermal-electrochemistry approach synergistic regulation catalytic processes, highlighting potential multifield-coupled advance sustainable-energy-powered chemical synthesis technologies.

Language: Английский

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Cu-Doped Iron Oxide for the Efficient Electrocatalytic Nitrate Reduction Reaction

Nano Letters, Journal Year: 2023, Volume and Issue: 23(5), P. 1897 - 1903

Published: Feb. 22, 2023

The electrochemical nitrate reduction reaction (NO3RR) is a promising alternative synthetic route for sustainable ammonia (NH3) production, because it not only eliminates (NO3-) from water but also produces NH3 under mild operating conditions. However, owing to the complicated eight-electron and competition hydrogen evolution reaction, developing catalysts with high activities Faradaic efficiencies (FEs) highly imperative improve performance. In this study, Cu-doped Fe3O4 flakes are fabricated demonstrated be excellent conversion of NO3- NH3, maximum FE ∼100% an yield 179.55 ± 16.37 mg h-1 mgcat-1 at -0.6 V vs RHE. Theoretical calculations reveal that doping catalyst surface Cu results in more thermodynamically facile reaction. These highlight feasibility promoting NO3RR activity using heteroatom strategies.

Language: Английский

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Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: May 19, 2023

Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions under ambient conditions is regarded as a sustainable development strategy to achieve carbon neutrality and high-value utilization of harmful substances. Herein, we report an process for selective synthesis high-valued formamide from monoxide nitrite with Ru1Cu single-atom alloy conditions, which achieves high selectivity Faradaic efficiency 45.65 ± 0.76% at -0.5 V vs. RHE. In situ X-ray absorption spectroscopy, coupled in Raman spectroscopy density functional theory calculations results reveal that the adjacent Ru-Cu dual active sites can spontaneously couple *CO *NH2 intermediates realize critical reaction, enabling high-performance electrosynthesis formamide. This work offers insight electrocatalysis CO NO2- paving way more-sustainable chemical products.

Language: Английский

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Tandem Nitrate‐to‐Ammonia Conversion on Atomically Precise Silver Nanocluster/MXene Electrocatalyst

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(8)

Published: Jan. 5, 2024

Abstract Electrocatalytic reduction of nitrate (NO 3 RR) to synthesize ammonia (NH ) provides a competitive manner for carbon neutrality and decentralized NH synthesis. Atomically precise nanoclusters, as an advantageous platform investigating the NO RR mechanisms actual active sites, remain largely underexplored due poor stability. Herein, we report 4 9 [Ag (mba) ] nanoclusters (Ag NCs) loaded on Ti C 2 MXene /MXene) highly efficient performance towards ambient synthesis with improved stability in neutral medium. The composite structure Ag NCs enables tandem catalysis process reduction, significantly increasing selectivity FE . Besides, compared individual NCs, /MXene has better current density performed no decay after 108 hours reaction. This work strategy improving catalytic activity atomically metal expanding mechanism research application NCs.

Language: Английский

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