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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Laser-controlled tandem catalytic sites of CuNi alloys with ampere-level electrocatalytic nitrate-to-ammonia reduction activities for Zn–nitrate batteries

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(7), P. 2991 - 3001

Published: Jan. 1, 2023

Laser-constructed CuNi alloy electrodes with tandem sites of Ni provide H* and Cu for NO 3 − reduction, achieving ampere-level reduction high-performance Zn–NO batteries.

Language: Английский

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A Bi‐Co Corridor Construction Effectively Improving the Selectivity of Electrocatalytic Nitrate Reduction toward Ammonia by Nearly 100%

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(48)

Published: Sept. 22, 2023

Improving the selective ammonia production capacity of electrocatalytic nitrate reduction reaction (NO3 RR) at ambient conditions is critical to future development and industrial application electrosynthesis ammonia. However, involves multi-proton electron transfer as well desorption underutilization intermediates, posing a challenge selectivity NO3 RR. Here electrodeposition site Co modulated by depositing Bi bottom catalyst, thus obtaining Co+Bi@Cu NW catalyst with Bi-Co corridor structure. In 50 mm NO3- , exhibits highest Faraday efficiency ≈100% (99.51%), an yield rate 1858.2 µg h-1 cm-2 high repeatability -0.6 V versus reversible hydrogen electrode. Moreover, change NO2- concentration on surface observed in situ reflection absorption imaging intermediates RR process detected electrochemical Raman spectroscopy together verify trapping effect It believed that measure modulating deposition loading element easy-to-implement general method for improving NH3 corresponding scientific research applications.

Language: Английский

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Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(14)

Published: Jan. 26, 2024

Abstract Electrocatalytic nitrate reduction reaction (NO 3 RR) toward ammonia synthesis is recognized as a sustainable strategy to balance the global nitrogen cycle. However, it still remains great challenge achieve highly efficient production due complex proton‐coupled electron transfer process in NO RR. Here, controlled of RuMo alloy nanoflowers (NFs) with unconventional face‐centered cubic (fcc) phase and hexagonal close‐packed/fcc heterophase for RR reported. Significantly, fcc NFs demonstrate high Faradaic efficiency 95.2% large yield rate 32.7 mg h −1 cat at 0 −0.1 V (vs reversible hydrogen electrode), respectively. In situ characterizations theoretical calculations have unraveled that possess highest d‐band center superior electroactivity, which originates from strong Ru─Mo interactions intrinsic activity phase. The optimal electronic structures supply adsorption key intermediates suppression competitive evolution, further determines remarkable performance. successful demonstration high‐performance zinc‐nitrate batteries suggests their substantial application potential electrochemical energy systems.

Language: Английский

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Unveiling the Reaction Mechanism of Nitrate Reduction to Ammonia Over Cobalt-Based Electrocatalysts

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(19), P. 12976 - 12983

Published: April 3, 2024

Electrocatalytic reduction of nitrate to ammonia (NRA) has emerged as an alternative strategy for sewage treatment and generation. Despite excellent performances having been achieved over cobalt-based electrocatalysts, the reaction mechanism well veritable active species across a wide potential range are still full controversy. Here, we adopt CoP, Co, Co3O4 model materials solve these issues. CoP evolves into core@shell structured CoP@Co before NRA. For Co catalysts, three-step relay is carried out superficial dynamical Coδ+ under low overpotential, while continuous hydrogenation from unveiled high overpotential. In comparison, stable steadily catalyze range. As result, exhibit much higher NRA activity than especially Moreover, performance although they experience same mechanism. A series characterizations clarify reason enhancement highlighting that core donates abundant electrons species, leading generation more hydrogen nitrogen-containing intermediates.

Language: Английский

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H* Species Regulation by Mn‐Co(OH)₂ for Efficient Nitrate Electro‐reduction in Neutral Solution

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)

Published: Jan. 23, 2024

Abstract During the electrocatalytic NO 3 − reduction reaction (NO RR) under neutral condition, activation of H 2 O to generate H* and inhibition inter‐H* species binding, are critically important but remain challenging for suppressing non‐desirable hydrogen evolution (HER). Here, a Mn‐doped Co(OH) (named as Mn‐Co(OH) ) has been synthesized by in situ reconstruction electrolyte, which is able dissociate molecules inhibits binding between each other owing increased interatomic spacing Mn‐doping. The electrocatalyst offers faradaic efficiency (FE) high 98.9±1.7% at −0.6 V vs. reversible electrode (RHE) an energy (EE) 49.90±1.03% NH production RR, among highest recently reported state‐of‐the‐art catalysts electrolyte. Moreover, negligible degradation −200 mA cm −2 found least 500 h, longest catalytic durations ever reported. This work paves novel approach design synthesis efficient RR electrocatalysts.

Language: Английский

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Relay Catalysis of Fe and Co with Multi‐Active Sites for Specialized Division of Labor in Electrocatalytic Nitrate Reduction Reaction

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

Published: April 8, 2024

Abstract Electrocatalytic nitrate reduction reaction (NO 3 RR) driven by renewable energy is a promising technology for the removal of nitrate‐containing wastewater. However, sluggish kinetics resulted from complex proton‐coupled electron transfer and various intermediates remain key barriers large‐scale application NO RR. Herein, tactic reported to raise rate RR increase selectivity N 2 using bimetal catalyst: Co inclined act on steps needed in process, rate‐determining step (RDS: *NO , asterisk means intermediates) subsequent *N hydrogenation as well Fe exhibits efficient activity selectivity‐ determining (SDS: then ) via relay catalysis mechanism. A efficiency 78.5% an ultra‐long cycle stability 60 cycles (12 h per cycle) are achieved FeCo alloy confined with nitrogen‐doped porous carbon nanofibers (FeCo‐NPCNFs). DFT calculations unveil that introduction active site not only regulates d‐band center alloy, optimizes adsorption intermediates, but also has strong capacity supply hydrogen species. Clearly, this study elucidates effects bimetallic performance electrocatalytic offers avenues designing Fe‐based catalysts realize nitrogen‐neutral cycle.

Language: Английский

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Strategies and applications of electrocatalytic nitrate reduction towards ammonia

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 506, P. 215723 - 215723

Published: Feb. 26, 2024

Language: Английский

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Regulating the d-Band Center of Metal–Organic Frameworks for Efficient Nitrate Reduction Reaction and Zinc-Nitrate Battery

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(21), P. 16205 - 16213

Published: Oct. 18, 2024

The electrochemical reduction of nitrate ions to valuable ammonia enables the recovery pollutants from industrial wastewater, thereby synchronously balancing nitrogen cycle and achieving NH3 production. However, currently reported electrocatalysts still suffer low yield rate, Faradaic inefficiency, partial current density. Herein, a strategy based on regulation d-band center by Ru doping is presented boost Theoretical calculations unravel that dopant in Ni metal–organic framework shifts neighboring sites upward, optimizing adsorption strength N-intermediates, resulting greatly enhanced reaction performance. synthesized Ru-doped rod array electrode delivers rate 1.31 mmol h–1 cm–2 efficiency 91.5% at −0.6 V versus reversible hydrogen electrode, as well good cycling stability. In view multielectron transfer electrocatalytic activity, Zn-NO3– battery assembled this Zn anode, which high open-circuit voltage 1.421 maximum output power density 4.99 mW cm–2, demonstrating potential application value.

Language: Английский

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Electrocatalytic upgrading of nitrogenous wastes into value-added chemicals: A review

Materials Today, Journal Year: 2024, Volume and Issue: 73, P. 208 - 259

Published: Feb. 7, 2024

Language: Английский

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