Recent Progress and Perspectives on Transition Metal-Based Electrocatalysts for Efficient Nitrate Reduction

Energy & Fuels, Journal Year: 2024, Volume and Issue: 38(8), P. 6701 - 6722

Published: April 8, 2024

Electrochemical nitrate reduction is the process of converting into ammonia or nitrogen using electric energy. This saves energy, protects environment, and an important technology for resource recovery water purification. paper examines recent advances in electrochemical research analyzes reaction mechanism path as well influence various factors on through thermodynamic kinetic principles. Second, catalytic performances transition metal electrocatalysts form single metals, alloys, oxides, composites are analyzed detail, which lays foundation rational development new, efficient, stable electrocatalysts. Finally, future directions prospects envisioned.

Language: Английский

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Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(18)

Published: March 7, 2024

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) is a promising and eco‐friendly strategy for production. However, the sluggish kinetics eight‐electron transfer process poor mechanistic understanding strongly impedes its application. To unveil internal laws, herein, library Pd‐based bimetallene with various transition metal dopants (PdM (M=Fe, Co, Ni, Cu)) are screened learn their structure–activity relationship towards NO RR. The ultra‐thin structure metallene greatly facilitates exposure active sites, metals break electronic balance upshift d‐band center, thus optimizing intermediates adsorption. anisotropic characteristics these make RR activity in order PdCu>PdCo≈PdFe>PdNi>Pd, record‐high NH yield rate 295 mg h −1 cat along Faradaic efficiency 90.9 % achieved neutral electrolyte on PdCu bimetallene. Detailed studies further reveal that moderate N‐species (*NO *NO 2 ) adsorption ability, enhanced activation, reduced HER facilitate We believe our results will give systematic guidance future design catalysts.

Language: Английский

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Recent advances of ammonia synthesis under ambient conditions over metal-organic framework based electrocatalysts

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123161 - 123161

Published: Aug. 10, 2023

Language: Английский

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Achieving Near 100% Faradaic Efficiency of Electrocatalytic Nitrate Reduction to Ammonia on Symmetry-Broken Medium-Entropy-Alloy Metallene

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 7907 - 7916

Published: May 6, 2024

Electrochemical nitrate reduction (NO3RR) offers an ecofriendly way for ammonia production. However, improving the sluggish kinetics of such a multistep reaction still remains challenging. Herein, asymmetry strategy is proposed to adjust charge distribution active centers on metallene by presenting novel symmetry-broken medium-entropy-alloy (MEA) via heteroatom alloying. Benefiting from maximized exposure well-regulated sites, proof-of-concept PdCuCo MEA delivers near 100% NH3 Faradaic efficiency in both neutral and alkaline electrolytes, along with record-high yield rate over 532.5 mg h–1 mgcat–1. Moreover, it enables 99.7% conversion industrial wastewater level 6200 ppm drinkable water level. Detailed studies further revealed that redistribution induced elemental electronegativity difference metallene, which will weaken N–O bond *NO, thus reducing energy barrier rate-determining step. Meanwhile, competitive HER formation NO2– are also hindered. We believe our this work shed light design efficient NO3RR catalysts more practical

Language: Английский

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Electrocatalysts with atomic-level site for nitrate reduction to ammonia

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 96, P. 642 - 668

Published: May 27, 2024

Language: Английский

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Defect and interface engineering for promoting electrocatalytic N-integrated CO2 co-reduction

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2024, Volume and Issue: 57, P. 1 - 17

Published: Feb. 1, 2024

Language: Английский

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Bi₁‐CuCo₂O₄ Hollow Carbon Nanofibers Boosts NH₃ Production from Electrocatalytic Nitrate Reduction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 6, 2024

Abstract Ammonia, as a high‐energy‐density carrier for hydrogen storage, is in great demand worldwide. Electrocatalytic nitrate reduction reaction (NO 3 RR) provides green NH production process. However, the complex pathways NO RR to and difficulty controlling intermediate products limit Herein, by incorporating atomic‐level bismuth (Bi) into CuCo 2 O 4 hollow carbon nanofibers, catalytic activity of electrocatalyst enhanced. The maximum Faradaic efficiency Bi 1 ‐CuCo 95.53%, with an yield 448.74 µmol h −1 cm −2 at −0.8 V versus RHE. Density Functional Theory calculations show that presence lowers barrier hydrogenation step from *NO H, while promoting mass transfer on release *NH reactivation surface‐active sites. Differential charge density also after doping, supplied catalyst − increases 0.62 0.72 e ‐ , thus reasoned enhanced activity. established nitrate‐Zn battery shows energy 2.81 mW implying potential application.

Language: Английский

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Core–Shell Engineering Boosted Active Hydrogen Generation in Cu_2–xS/MoS₂ Quantum Dots for Efficient Electrocatalytic Nitrate Reduction to Ammonia

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(15), P. 5979 - 5990

Published: April 1, 2024

The electrochemical nitrate reduction reaction (NO3RR) emerges as a promising method for ammonia (NH3) production, which faces the dilemma of inhibiting hydrogen evolution (HER) and promoting active (Hads) supply hydrogenation nitrogen intermediates. Here, core–shell structure engineering strategy is developed Cu2–xS/MoS2, where strong Hads adsorption storage capacity can accelerate As result, an eminent NH3 yield 0.178 mmol h–1 cm–2 Faradaic efficiency 84.5% were achieved. A series tests demonstrate that tuning Cu2–xS/MoS2 interface improve activity conversion NO2–, while avoiding HER effectively retain Hads. density functional theory calculation further demonstrates has *H retention ability to promote NO3RR process. This work offers novel perspective on manipulation generation NO3RR.

Language: Английский

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Boron‐Doped Ti₃C₂T_x MXene for Effective and Durable High‐Current‐Density Ammonia Synthesis

Small, Journal Year: 2024, Volume and Issue: 20(45)

Published: July 24, 2024

Abstract Ammonia (NH 3 ) synthesis via the nitrate reduction reaction (NO RR) offers a competitive strategy for nitrogen cycling and carbon neutrality; however, this is hindered by poor NO RR performance under high current density. Herein, it shown that boron‐doped Ti C 2 T x MXene nanosheets can highly efficiently catalyze conversion of RR‐to‐NH at ambient conditions, showing maximal NH Faradic efficiency 91% with peak yield rate 26.2 mgh −1 mg cat. , robust durability over ten consecutive cycles, all them are comparable to best‐reported results exceed those pristine MXene. More importantly, when tested in flow cell, designed catalyst delivers density ‒1000 mA cm −2 low potential ‒1.18 V versus reversible hydrogen electrode maintains selectivity wide range. Besides, Zn–nitrate battery as cathode assembled, which achieves power 5.24 mW 1.15 . Theoretical simulations further demonstrate boron dopants optimize adsorption activation intermediates, reduce potential‐determining step barrier, thus leading an enhanced selectivity.

Language: Английский

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Metal/covalent-organic framework-based electrocatalysts for electrochemical reduction of nitrate to ammonia

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 518, P. 216061 - 216061

Published: July 8, 2024

The pervasive contamination of industrial, domestic, and agricultural wastewater with nitrate poses profound ecological public health risks. Traditional methods for remediating nitrate-laden water face formidable challenges due to its high solubility stability. However, a promising solution emerges in the form electrochemical reduction (eNO3RR), offering both efficient removal valuable ammonia generation sustainable manner. This review explores burgeoning field eNO3RR, focusing on recent advancements utilizing porous crystalline framework materials − metal–organic frameworks (MOFs) covalent-organic (COFs) as novel class electrocatalysts. These innovative exhibit unique properties such adjustable porosity, diverse structures, tunable pore sizes, well-defined active sites, making them ideal candidates enhancing efficiency selectivity under ambient conditions. By dissecting structure–activity relationship inherent MOF/COF-based electrocatalysts, this aims provide comprehensive understanding their role driving conversion NO3− NH3. Moreover, it identifies current proposes future prospects leveraging these advanced pollutants, glimpse into greener more effective approach remediation resource recovery.

Language: Английский

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