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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Boosting Electrocatalytic Nitrate Reduction to Ammonia via Promoting Water Dissociation

ACS Catalysis, Год журнала: 2023, Номер 13(16), С. 10846 - 10854

Опубликована: Авг. 2, 2023

Electrocatalytic nitrate reduction reaction (NO3–RR) opens opportunities for ammonia production. The sluggish kinetics of this multielectron and multiproton process has been regarded as the key issue. Herein, we report a Cu1Co5 alloy electrocatalytic NO3–RR to NH3. It achieves high current density (453 mA cm–2) Faradaic efficiency (96.2%) NH3 production at 0.075 V vs RHE, with half-cell energy 44.9%, higher than those Cu, Co, other Co-based alloys, is among highest value reported. We found that interaction between Cu Co reorganizes their electronic structure in alloys. NO3– adsorption switches spontaneous process, *NO → *N *NH *NH2 processes are promoted. Importantly, water dissociation concerted transformation N-species proven be rate-determining, which facilitated on sites essential enhanced NO3–RR. This inspires us strategy designing more efficient catalysts under alkaline condition by promoting H2O process.

Язык: Английский

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Modulating the Active Hydrogen Adsorption on Fe─N Interface for Boosted Electrocatalytic Nitrate Reduction with Ultra‐Long Stability

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Июль 25, 2023

The electrocatalytic reduction of nitrate (NO3- ) to nitrogen (N2 is an environmentally friendly approach for efficient N-cycle management (toward a nitrogen-neutral cycle). However, poor catalyst durability and the competitive hydrogen evolution reaction significantly impede its practical application. Interface-chemistry engineering, utilizing close relationship between surface/interface microenvironment electron/proton transfer process, has facilitated development catalysts with high intrinsic activity physicochemical durability. This study reports synthesis nitrogen-doped carbon-coated rice-like iron nitride (RL-Fe2 N@NC) electrocatalyst excellent nitrate-reduction (high N2 selectivity (≈96%) NO3- conversion (≈86%)). According detailed mechanistic investigations by in situ tests theoretical calculations, strong hydrogenation ability enhanced enrichment system synergistically contribute rapid nitrogen-containing species, increasing reducing occurrence competing hydrogen-evolution side reaction. Moreover, RL-Fe2 N@NC shows stability, retaining good -to-N2 electrocatalysis more than 40 cycles (one cycle per day). paper could guide interfacial design Fe-based composite nanostructures reduction, facilitating shift toward neutrality.

Язык: Английский

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Electrocatalytic reduction of nitrate to ammonia on low-cost manganese-incorporated Co3O4 nanotubes

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 324, С. 122293 - 122293

Опубликована: Дек. 16, 2022

Язык: Английский

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Interfacial Engineering of Bimetallic Ni/Co-MOFs with H-Substituted Graphdiyne for Ammonia Electrosynthesis from Nitrate

ACS Nano, Год журнала: 2023, Номер 17(7), С. 6687 - 6697

Опубликована: Март 17, 2023

The electrochemical synthesis of ammonia is highly dependent on the coupling reaction between nitrate and water, for which an electrocatalyst with a multifunctional interface anticipated to promote deoxygenation hydrogenation water. Herein, by engineering surface bimetallic Ni/Co-MOFs (NiCoBDC) hydrogen-substituted graphdiyne (HsGDY), hybrid nanoarray NiCoBDC@HsGDY has been achieved toward scale-up nitrate-to-ammonia conversion. On one hand, partial electron transfers from Ni2+ coordinatively unsaturated Co2+ NiCoBDC, not only promotes *NO3 but also activates water-dissociation *H Ni2+. other conformal coated HsGDY facilitates both electrons NO3- ions gathering NiCoBDC HsGDY, moves forward rate-determining step *N *H2O Co2+. As result, such delivers high NH3 yield rates Faradaic efficiency above 90% over wide potential pH windows. When assembled into galvanic Zn-NO3- battery, power density 3.66 mW cm-2 achieved, suggesting its in area aqueous Zn-based batteries.

Язык: Английский

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Single Atom Environmental Catalysis: Influence of Supports and Coordination Environments

Advanced Functional Materials, Год журнала: 2023, Номер 33(50)

Опубликована: Авг. 27, 2023

Abstract Single‐atom catalysts (SACs) are desirable in environmental catalysis due to friendliness, structural stability, and maximum utilization of active metal sites. Extensive research has compared the catalytic performance between SACs with different single‐atom metals. However, their is also highly dependent on supports, which play an important role modulating local coordination environment SACs. Unfortunately, a comprehensive review that systematically discusses relationship supports environment, as well combined effects scare. In this review, three widely investigated applications including advanced oxidation processes (AOPs), mainly Fenton Fenton‐like reactions, nitrate reduction reaction (NO 3 RR) focused. By correlating characterization results, performances, computational environments reactivity examined detail, from origin pathways AOPs NO RR attempted reveal. Finally look forward for potential opportunities challenges on‐demand applications, provided.

Язык: Английский

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Intermediates Regulation via Electron‐Deficient Cu Sites for Selective Nitrate‐to‐Ammonia Electroreduction

Advanced Materials, Год журнала: 2023, Номер 35(48)

Опубликована: Сен. 21, 2023

Ammonia (NH3 ), known as one of the fundamental raw materials for manufacturing commodities such chemical fertilizers, dyes, ammunitions, pharmaceuticals, and textiles, exhibits a high hydrogen storage capacity ≈17.75%. Electrochemical nitrate reduction (NO3 RR) to valuable ammonia at ambient conditions is promising strategy facilitate artificial nitrogen cycle. Herein, copper-doped cobalt selenide nanosheets with selenium vacancies are reported robust highly efficient electrocatalyst ammonia, exhibiting maximum Faradaic efficiency ≈93.5% an yield rate 2360 µg h-1 cm-2 -0.60 V versus reversible electrode. The in situ spectroscopical theoretical study demonstrates that incorporation Cu dopants Se into efficiently enhances electron transfer from Co atoms via bridging atoms, forming electron-deficient structure sites accelerate NO3- dissociation stabilize *NO2 intermediates, eventually achieving selective catalysis entire NO3 RR process produce efficiently.

Язык: Английский

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Nickel-facilitated in-situ surface reconstruction on spinel Co3O4 for enhanced electrochemical nitrate reduction to ammonia

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 340, С. 123219 - 123219

Опубликована: Авг. 24, 2023

Язык: Английский

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Enhanced electrocatalytic nitrate reduction through phosphorus-vacancy-mediated kinetics in heterogeneous bimetallic phosphide hollow nanotube array

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 330, С. 122627 - 122627

Опубликована: Март 14, 2023

Язык: Английский

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Palladium-Copper bimetallic catalysts for electroreduction of CO2 and nitrogenous species

Coordination Chemistry Reviews, Год журнала: 2024, Номер 509, С. 215802 - 215802

Опубликована: Март 26, 2024

Язык: Английский

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