Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction

Chem, Journal Year: 2023, Volume and Issue: 9(7), P. 1768 - 1827

Published: June 21, 2023

Language: Английский

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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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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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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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Boosting Electrocatalytic Nitrate Reduction to Ammonia via Promoting Water Dissociation

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(16), P. 10846 - 10854

Published: Aug. 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.

Language: Английский

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Efficient bubble/precipitate traffic enables stable seawater reduction electrocatalysis at industrial-level current densities

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 5, 2024

Abstract Seawater electroreduction is attractive for future H 2 production and intermittent energy storage, which has been hindered by aggressive Mg 2+ /Ca precipitation at cathodes consequent poor stability. Here we present a vital microscopic bubble/precipitate traffic system (MBPTS) constructing honeycomb-type 3D robust anti-precipitation seawater reduction (SR), massively/uniformly release small-sized bubbles to almost every corner of the cathode repel precipitates without break. Noticeably, optimal with built-in MBPTS not only enables state-of-the-art alkaline SR performance (1000-h stable operation –1 A cm −2 ) but also highly specialized in catalytically splitting natural into greatest ability. Low amounts after prolonged tests under large current densities reflect genuine efficacy our MBPTS. Additionally, flow-type electrolyzer based on stably functions industrially-relevant 500 mA 150 h while unwaveringly sustaining near-100% Faradic efficiency. Note that estimated price (~1.8 US$/kg H2 even cheaper than US Department Energy’s goal (2 ).

Language: Английский

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Atomic coordination environment engineering of bimetallic alloy nanostructures for efficient ammonia electrosynthesis from nitrate

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(32)

Published: July 31, 2023

Electrochemical nitrate reduction reaction (NO 3 RR) to ammonia has been regarded as a promising strategy balance the global nitrogen cycle. However, it still suffers from poor Faradaic efficiency (FE) and limited yield rate for production on heterogeneous electrocatalysts, especially in neutral solutions. Herein, we report one-pot synthesis of ultrathin nanosheet-assembled RuFe nanoflowers with low-coordinated Ru sites enhance NO RR performances electrolyte. Significantly, exhibit outstanding FE 92.9% 38.68 mg h −1 cat (64.47 ) at −0.30 −0.65 V (vs. reversible hydrogen electrode), respectively. Experimental studies theoretical calculations reveal that are highly electroactive an increased d-band center guarantee efficient electron transfer, leading low energy barriers reduction. The demonstration rechargeable zinc-nitrate batteries large-specific capacity using indicates their great potential next-generation electrochemical systems.

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

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(46)

Published: July 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.

Language: Английский

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Boosting Electrocatalytic Nitrate‐to‐Ammonia via Tuning of N‐Intermediate Adsorption on a Zn−Cu Catalyst

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: Sept. 4, 2023

The renewable-energy-powered electroreduction of nitrate (NO3- ) to ammonia (NH3 has garnered significant interest as an eco-friendly and promising substitute for the Haber-Bosch process. However, sluggish kinetics hinders its application at a large scale. Herein, we first calculated N-containing species (*NO3 *NO2 binding energy free hydrogen evolution reaction over Cu with different metal dopants, it was shown that Zn candidate. Based on theoretical study, designed synthesized Zn-doped nanosheets, as-prepared catalysts demonstrated excellent performance in NO3- -to-NH3 . maximum Faradaic efficiency (FE) NH3 could reach 98.4 % outstanding yield rate 5.8 mol g-1 h-1 , which is among best results up date. catalyst also had cycling stability. Meanwhile, presented FE exceeding 90 across wide potential range concentration range. Detailed experimental studies revealed doping modulate intermediates adsorption strength, enhance NO2- conversion, change *NO configuration bridge adsorption, decrease barrier, leading catalytic

Language: Английский

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