Enhancing Compatibility of Two‐Step Tandem Catalytic Nitrate Reduction to Ammonia Over P‐Cu/Co(OH)₂

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

Published: Sept. 11, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to realize ammonia generation and wastewater treatment. However, the transformation from NO − NH involves multiple proton‐coupled electron transfer processes by‐products 2 , H etc.), making high selectivity challenge. Herein, two‐phase nanoflower P‐Cu/Co(OH) electrocatalyst consisting of P‐Cu clusters P‐Co(OH) nanosheets designed match two‐step tandem process ) more compatible, avoiding excessive accumulation optimizing whole reaction. Focusing on initial 2e process, inhibited * desorption Cu sites in gives rise appropriate released electrolyte. Subsequently, exhibits superior capacity for trapping transforming desorbed during latter 6e due thermodynamic advantage contributions active hydrogen. In 1 m KOH + 0.1 leads yield rate 42.63 mg h cm Faradaic efficiency 97.04% at −0.4 V versus reversible hydrogen electrode. Such well‐matched achieves remarkable synthesis performance perspective catalytic reaction, offering novel guideline design RR electrocatalysts.

Language: Английский

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A Porous Copper Catalyst for Electrochemical Nitrate Reduction to Ammonium

Journal of environmental chemical engineering, Journal Year: 2025, Volume and Issue: unknown, P. 115596 - 115596

Published: Jan. 1, 2025

Language: Английский

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Self-Triggering a Locally Alkaline Microenvironment of Co₄Fe₆ for Highly Efficient Neutral Ammonia Electrosynthesis

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 28, 2025

Electrochemical nitrate reduction reaction (eNO3-RR) to ammonia (NH3) holds great promise for the green treatment of NO3- and ambient NH3 synthesis. Although Fe-based electrocatalysts have emerged as promising alternatives, their excellent eNO3-RR-to-NH3 activity is usually limited harsh alkaline electrolytes or alloying noble metals with Fe in sustainable neutral electrolytes. Herein, we demonstrate an unusual self-triggering localized alkalinity Co4Fe6 electrocatalyst efficient media, which breaks down conventional pH-dependent kinetics restrictions shows a 98.6% Faradaic efficiency (FE) 99.9% selectivity at -0.69 V vs RHE. The synergetic Co-Fe dual sites were demonstrated enable optimal free energies species balance water dissociation protonation adsorbed NO2-. Notably, can attain high current density 100 mA cm-2 FE surpassing 96% long-term stability over 500 h membrane electrode assembly (MEA) electrolyzer. This work provides insight into tailoring self-reinforced local-alkalinity on alloy thus avoids practical upcycling technology.

Language: Английский

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Nanoflower‐Like CuPd/CuO Heterostructure for an Energy‐Output Electrocatalytic System Coupling Ammonia Electrosynthesis and Zinc‐Nitrate Battery

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 18, 2025

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) can effectively alleviate pollution and simultaneously realize ammonia electrosynthesis at room temperature. However, it remains a significant challenge for NO RR to achieve high Faradic efficiency in full concentration range. Herein, nanoflower‐like copper‐palladium alloy/CuO heterostructure (CuPd/CuO@NF) is successfully fabricated by the hydrothermal synthesis of CuO nanoflowers subsequent formation CuPd alloy. The as‐obtained CuPd/CuO@NF exhibits remarkable electrochemical performance − ‐N range from 20 1400 ppm, especially with conversion rate 97.8% NH selectivity 99.3% 94.2% yield 1.37 mmol h −1 cm −2 ppm. In‐situ Fourier transform infrared spectroscopy Raman spectra reveal that first catalyzes 2 , which rapidly reduced forming *NH, *NH OH intermediates. Density functional theory calculations suggest NHO route thermodynamically favorable. When applied zinc‐nitrate battery, demonstrates maximum power density 53.7 mW 99.9% 94.4%. This work offers valuable insights into design novel electrocatalysts batteries.

Language: Английский

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Interface Engineering on Heterostructural Nanosheets for Efficient Electrocatalytic-Paired Upcycling of Waste Plastics and Nitrate

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 18095 - 18106

Published: Nov. 22, 2024

Language: Английский

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Engineering Ce Promoter to Regulate H^* Species to Boost Tandem Electrocatalytic Nitrate Reduction for Ammonia Synthesis

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Abstract The renewable‐energy‐powered electroreduction of nitrate (NO 3 RR) to ammonia emerges as a generalist for contamination remediation, green synthesis, and even advanced energy conversion, garnering significant interest. However, it comes across limited yield selectivity due the imbalance active hydrogen (H * ) supply within cutting‐edge single‐center Cu‐based materials. Herein, secondary Ce entity is engineered into Cu/MoO 2 @C substrate by thermal treatment Ce‐doping NENU‐5 precursors provide H effectively. A high NH rate (20.3 ± 0.7 mg h −1 cat. NO − −to−NH Faradaic efficiency (92 3%) at −0.4 V (vs RHE) can be reached in 5%Ce‐Cu/MoO @C, ranking among recently reported state‐of‐the‐art catalysts. core this boosting performance lies dual‐site tandem catalysis, which Cu site adsorbs activates , dissociates water generate respectively. And spillover from vicinal x intermediates on promotes hydrogenation generation with selectivity. Theoretical calculations further indicate that engineering optimizes electronic properties, activation adsorbed decreases barrier rate‐determining step catalysis. These findings consolidate positive role rare earth center highlight its corresponding catalysis sustainable synthesis.

Language: Английский

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Dichalcogenides as Emerging Electrocatalysts for Efficient Ammonia Synthesis: A Focus on Mechanisms and Theoretical Potentials

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 28, 2025

Abstract Developing sustainable technologies for ammonia production through electrochemical reactions offers a promising alternative by leveraging renewable energy sources to produce under ambient conditions. These methods include nitrogen reduction reaction (NRR), nitric oxide (NORR), nitrite (NO 2 RR), and nitrate 3 RR). Optimizing efficiency (EE) in synthesis has become increasingly crucial as commercialization approaches. Herein, this work comprehensive study of system EE improvements the theoretical voltage calculations based on pH expansion bifunctional catalysts like transition metal dichalcogenides (TMDs), which can efficiently catalyze oxygen evolution (OER) synthesis. The review summarizes pH‐dependent redox potential Pourbaix diagrams NRR, NO RR, offering insights into potential‐pH regions where oxides are reduced NH . Incorporating design enables researchers minimize losses better improve overall performance. Finally, wraps up exploring roles TMD different mechanisms identifying areas improvement. broader impact lies its transform alignment with global efforts reduce greenhouse gas emissions.

Language: Английский

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Revealing the Tandem Behavior of Iron‐Group/Copper Binary Catalysts in the Electroreduction of Nitrate to Ammonia

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 16, 2025

Abstract As a green strategy for both ammonia (NH 3 ) production and wastewater purification, electrochemical reduction of nitrate (NO RR) faces challenges due to the nitrite 2 − accumulation competitive hydrogen evolution reaction (HER). Tandem catalysis NO NH offers great potential enhancing selectivity. Herein, iron‐group (Fe, Co, or Ni) nanosheets are introduced onto Cu nanowires construct Cu‐Fe, Cu‐Co, Cu‐Ni tandem systems respectively. Specifically, sites facilitate conversion . Fe sites, similar Cu, reduce , exacerbating rather than converting it their inability precisely capture Co exhibiting excellent moderate HER activity, can seamlessly operate with realize well‐ordered relay catalysis, which achieves superior yield rate 48.44 mg h −1 cm −2 Ni demonstrate removal capability at low overpotentials, leading Faraday efficiency 99.47%. However, its remarkable HER‐active property demonstrated via in situ polarization imaging makes challenge ampere‐level current densities. This work identifies behavior coupled providing reference design further optimization system.

Language: Английский

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Catalyst–Support Interaction in Polyaniline-Supported Ni3Fe Oxide to Boost Oxygen Evolution Activities for Rechargeable Zn-Air Batteries

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Sept. 21, 2024

Catalyst-support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction (OER). Here we modulate catalyst-support polyaniline-supported Ni

Language: Английский

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Regulating Local Electron Distribution of Cu Electrocatalyst via Boron Doping for Boosting Rapid Absorption and Conversion of Nitrate to Ammonia

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(48)

Published: Oct. 15, 2024

Abstract The electrochemical reduction of nitrate to ammonia (NO 3 RR) is an effective route synthesis with the characteristics low energy input. However, complex multi‐electron/proton transfer pathways associated this reaction may trigger accumulation competitive by‐products. Herein, boron (B)‐doped Cu electrode (denoted as B–Cu 2 O/Cu/CP) “all‐in‐one” catalyst prepared by one‐step electrodeposition strategy. Caused B doping, charge redistribution and local coordination environment O/Cu species are modulated, resulting in exposure active sites on O/Cu/CP catalyst. In‐situ Fourier transform infrared spectroscopy theoretical investigations demonstrate that both O modulated can effectively enhance adsorption NO − facilitate conversion intermediate by‐products, thus promoting direct NH . Consequently, a remarkable Faradaic efficiency 92.74% be obtained minimal It expected work, based heterogeneous will open maneuverable versatile way for design catalysts.

Language: Английский

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