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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Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides

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

Published: Jan. 4, 2024

Abstract The electrochemical conversion of nitrate to ammonia is a way eliminate pollutant in water. Cu-Co synergistic effect was found produce excellent performance generation. However, few studies have focused on this high-entropy oxides. Here, we report the spin-related nitrate-to-ammonia using oxide Mg 0.2 Co Ni Cu Zn O. In contrast, Li-incorporated MgCoNiCuZnO exhibits inferior performance. By correlating electronic structure, that spin states are crucial for pair with high O can facilitate generation, while low decreases These findings offer important insights employing and inside selective catalysis. It also indicates generality magnetic synthesis between electrocatalysis thermal

Language: Английский

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Elucidating the Intrinsic Activity and Selectivity of Cu for Nitrate Electroreduction

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(9), P. 3658 - 3665

Published: Aug. 4, 2023

Cu-based catalysts have been widely explored for the electrochemical nitrate reduction reaction (NO3RR), while intrinsic activity and selectivity of Cu metal NO3RR remain ambiguous, preventing a genuine comparison performance. Here we use polycrystalline foils benchmarking elucidate impact often overlooked factors on NO3RR, including facet exposure, concentration, electrode surface area. An electropolished foil exhibits higher to NH3 than wet-etched foil, benefiting from greater exposure Cu(100) facets that are more favorable NO3RR. While shows no apparent dependence it increases monotonically with area, which is attributed promoted conversion intermediately produced NO2– larger electrode, as validated by 15N isotope labeling experiment. Our work provides mechanistic insights toward rational design electrocatalysts.

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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Synergistic Effect of Ni/Ni(OH)₂ Core‐Shell Catalyst Boosts Tandem Nitrate Reduction for Ampere‐Level Ammonia Production

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Electrocatalytic reduction of nitrate to ammonia provides a green alternate the Haber-Bosch method, yet it suffers from sluggish kinetics and low yield rate. The follows tandem reaction nitrite subsequent hydrogenation generate ammonia, Faraday efficiency (FE) is limited by competitive hydrogen evolution reaction. Herein, we design heterostructure catalyst remedy above issues, which consists Ni nanosphere core Ni(OH)

Language: Английский

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Atomic-Scale Tailoring C–N Coupling Sites for Efficient Acetamide Electrosynthesis over Cu-Anchored Boron Nitride Nanosheets

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 4, 2024

Electrochemical conversion of carbon and nitrogen sources into valuable chemicals provides a promising strategy for mitigating CO

Language: Английский

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Rethinking nitrate reduction: redirecting electrochemical efforts from ammonia to nitrogen for realistic environmental impacts

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(8), P. 2682 - 2685

Published: Jan. 1, 2024

Electrochemical NO 3 − reduction to NH is insignificant for practical applications. Instead, contaminants should be converted into N 2 , recycled chemicals, or coupled with CO produce value-added fertilizers if applicable.

Language: Английский

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Red Carbon Mediated Formation of Cu₂O Clusters Dispersed on the Oxocarbon Framework by Fehling's Route and their Use for the Nitrate Electroreduction in Acidic Conditions

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: March 26, 2024

Abstract The oligomers of carbon suboxide, known as red carbon, exhibit a highly conjugated structure and semiconducting properties. Upon mild heat treatment, it transforms into carbonaceous framework rich in oxygen surface terminations, called oxocarbon. In this study, the abundant functionalities are harnessed anchors to create oxocarbon‐supported nanohybrid electrocatalysts. Starting with single atomic Cu (II) strongly coordinated atoms on Fehling reaction leads formation 2 O clusters. Simultaneously, covalent oxocarbon emerges via cross‐linking, providing robust support for Notably, effectively stabilizes clusters very small size, ensuring their high durability acidic conditions presence ammonia. synthesized material exhibits superior electrocatalytic activity nitrate reduction under electrolyte conditions, yield rate ammonium (NH 4 + ) at 3.31 mmol h −1 mg cat Faradaic efficiency 92.5% potential −0.4 V (vs RHE).

Language: Английский

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Homogeneously Mixed Cu–Co Bimetallic Catalyst Derived from Hydroxy Double Salt for Industrial-Level High-Rate Nitrate-to-Ammonia Electrosynthesis

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(40), P. 27417 - 27428

Published: Aug. 23, 2024

Electrocatalytic nitrate reduction reaction (NO

Language: Английский

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Surface Engineering on Ag-Decorated Co₃O₄ Electrocatalysts for Boosting Nitrate Reduction to Ammonia

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11231 - 11242

Published: July 12, 2024

Electrochemical nitrate reduction reaction (NO3–RR) offers an alternative pathway toward ambient ammonia production and nitrogen balance restoration, requiring efficient catalysts. In this study, a silver-decorated cobalt oxide (Ag–Co3O4) catalyst was shown to enhance during NO3–RR in alkaline electrolyte. Specifically, the Ag–Co3O4 delivers (NH3) yield rate of 52 μmol h–1 cm–2 with Faradaic efficiency 88% at −0.32 V versus RHE. The activity is 6 times higher than that conventional Co3O4 (8.8 cm–2). catalytic selectivity originate from interaction between atomically dispersed Ag Co3O4, resulting formation active octahedral Co2+ species (Co2+Oh) unpaired eg electron, which facilitates activation adsorption NO3– ion promotes *NO2 adsorption, along its transformation *NO intermediate. This leads NH4+ production, as evidenced by combined experimental theoretical studies.

Language: Английский

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