Reconstruction-induced NiCu-based catalysts towards paired electrochemical refining

Energy & Environmental Science, Год журнала: 2022, Номер 15(7), С. 3004 - 3014

Опубликована: Янв. 1, 2022

A paired electrochemical refinery for simultaneously producing value-added ammonium and formate is successfully demonstrated using reconstruction-induced NiCu-based nanocomposites as both cathode anode electrocatalysts.

Язык: Английский

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Electrocatalytic nitrate-to-ammonia conversion with ~100% Faradaic efficiency via single-atom alloying

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 316, С. 121683 - 121683

Опубликована: Июнь 27, 2022

Язык: Английский

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

Inorganic Chemistry Frontiers, Год журнала: 2023, Номер 10(12), С. 3489 - 3514

Опубликована: Янв. 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.

Язык: Английский

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Iron Nanoparticles Protected by Chainmail‐structured Graphene for Durable Electrocatalytic Nitrate Reduction to Nitrogen

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(5)

Опубликована: Дек. 5, 2022

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is an appealing technology for regulating the nitrogen cycle. Metallic iron one of well‐known electrocatalysts NO RR, but it suffers from poor durability due to leaching and oxidation during electrocatalytic process. In this work, a graphene‐nanochainmail‐protected nanoparticle (Fe@Gnc) electrocatalyst reported. It displays superior removal efficiency high selectivity. Notably, catalyst delivers exceptional stability durability, with rate selectivity remained ≈96 % that first time after up 40 cycles (24 h cycle). As expected, conductive graphene nanochainmail provides robust protection internal active sites, allowing Fe@Gnc maintain its long‐lasting catalytic activity. This research proposes workable solution scientific challenge lasting ability iron‐based in large‐scale industrialization.

Язык: 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, Год журнала: 2023, Номер 16(6), С. 2483 - 2493

Опубликована: Янв. 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.

Язык: Английский

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Iron‐Based Nanocatalysts for Electrochemical Nitrate Reduction

Small Methods, Год журнала: 2022, Номер 6(10)

Опубликована: Сен. 14, 2022

Abstract Nitrate has a high level of stability and persistence in water, endangering human health aquatic ecosystems. Due to its reliability efficiency, the electrochemical nitrate reduction reaction (NO 3 RR) is regarded as best available option for mitigating excess water wastewater, especially removal trace levels nitrate. One most critical factors are catalysts, which directly affect efficiency removal. Iron‐based nanocatalysts, have advantages nontoxicity, wide availability, low cost, emerged promising NO RR material recent years. This review covers major aspects iron‐based nanocatalysts RR, including synthetic methods, structural design, performance enhancement, electrocatalytic test, mechanism. The progress mechanism functional modified structures reviewed from perspectives loading, doping, assembly strategies, order realize conversion pollutant harmless nitrogen or ammonia other sustainable products. Finally, challenges future directions development low‐cost highly‐efficient explored.

Язык: Английский

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Energy-efficient electrochemical ammonia production from dilute nitrate solution

Energy & Environmental Science, Год журнала: 2023, Номер 16(2), С. 663 - 672

Опубликована: Янв. 1, 2023

Highly efficient electrochemical nitrate reduction could be key for sustainable ammonia production. Our NiFe LDH/Cu foam electrode exhibits an NH 3 selectivity of 95.8% with 98.5% conversion.

Язык: Английский

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Metastable Phase Cu with Optimized Local Electronic State for Efficient Electrocatalytic Production of Ammonia from Nitrate

Advanced Functional Materials, Год журнала: 2022, Номер 33(6)

Опубликована: Ноя. 28, 2022

Abstract Electrocatalytic nitrate (NO 3 − ) reduction reaction (NITRR) is an inspiring route for ammonia (NH synthesis at ambient condition. The metallic Cu‐based material with low cost and high activity one of the most promising electrocatalysts NITRR. However, due to weaker atomic H * ‐providing capacity, produced intermediate—nitrite tends accumulate on its surface, leading unsatisfactory NH selectivity Faradic efficiency (FE). Herein, a novel facile O 2 /Ar plasma oxidation subsequent electro‐reduction strategy developed synthesize kind metastable phase Cu. Excitingly, Cu demonstrates superior NITRR performance conventional 4 + (97.8%) FE (99.8%). Density function theory (DFT) calculations reveal that upshift d ‐band center near Fermi level in contributes enhanced activity, while relatively strong adsorption facilitates conversion from NO /NO NOOH /NOH thus ensures FE. Furthermore, when evaluated as cathode Zn‐NO battery, power density (7.56 mW cm −2 yield (76 µmol h −1 are achieved by battery.

Язык: Английский

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Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

Advanced Materials, Год журнала: 2023, Номер 35(24)

Опубликована: Фев. 17, 2023

Ammonia is an indispensable commodity in the agricultural and pharmaceutical industries. Direct nitrate-to-ammonia electroreduction a decentralized route yet challenged by competing side reactions. Most catalysts are metal-based, metal-free with high conversion activity rarely reported. Herein, it shown that amorphous graphene synthesized laser induction comprising strained disordered pentagons, hexagons, heptagons can electrocatalyze eight-electron reduction of NO3- to NH3 Faradaic efficiency ≈100% ammonia production rate 2859 µg cm-2 h-1 at -0.93 V versus reversible hydrogen electrode. X-ray pair-distribution function analysis electron microscopy reveal unique molecular features facilitate reduction. In situ Fourier transform infrared spectroscopy theoretical calculations establish critical role these stabilizing reaction intermediates via structural relaxation. The enhanced catalytic enables implementation flow electrolysis for on-demand synthesis release >70% selectivity, resulting significantly increased yields survival rates when applied plant cultivation. results this study show significant promise remediating nitrate-polluted water completing NOx cycle.

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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