Heterogeneous β-Co(OH)2/Cu2(OH)3Cl bifunctional electrocatalyst for superior concurrent conversion of glycerol and nitrite

Journal of Energy Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Language: Английский

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Electro‐Reconstructed Transition Metal Electrodes for Coupled‐Upgrading of Nitrate Pollution and Waste Poly(Ethylene Terephthalate) Plastics

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

Published: Jan. 28, 2025

Abstract Two unrelated forms of pollution, nitrate‐containing wastewater and waste poly(ethylene terephthalate) (PET) plastics, can be converted into high‐value chemicals by electrochemical reduction oxidation reactions. Herein, coupled electrocatalysis is used for the co‐production ammonia (NH 3 ) formic acid (FA) with a cathode formed reconstructing Co on copper foam (R‐Co/CF) as catalyst nitrate reaction (NO RR) an anode NiCo nickel (R‐NiCo/NF) ethylene glycol (EGOR). The Faraday efficiency R‐Co/CF 96.2% that R‐NiCo/NF catalysts 98.2%. By coupling NO RR PET hydrolysate reaction, cell voltage required at current density 50 mA cm −2 202 mV lower than traditional electrolytic system, indicating electrocatalytic upcycling plastics energy‐saving cost‐effective strategy producing value‐added chemicals. Techno‐economic analysis indicates compared RR//OER RR//PET system save 2.8 × 10 kW h −1 in electricity generate ≈6 900 USD revenue per tonne NH .

Language: Английский

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Lattice Oxygen-Driven Co-Adsorption of Carbon Dioxide and Nitrate on Copper: A Pathway to Efficient Urea Electrosynthesis

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

Published: Feb. 10, 2025

The electrochemical coupling of CO2 and NO3– on copper-based catalysts presents a sustainable strategy for urea production while simultaneously addressing wastewater denitrification. However, the inefficient random adsorption copper surface limits interaction key carbon nitrogen intermediates, thereby impeding efficient C–N coupling. In this study, we demonstrate that residual lattice oxygen in oxide-derived nanosheets (OL-Cu) can effectively tune electron distribution, thus activating neighboring atoms generating electron-deficient (Cuδ+) sites. These Cuδ+ sites enhance stabilize *CO which enables directional at adjacent This mechanism shortens pathway achieves yield up to 298.67 mmol h–1 g–1 −0.7 V versus RHE, with an average Faradaic efficiency 31.71% high current density ∼95 mA cm–2. situ spectroscopic measurements confirmed formation tracked evolution intermediates (i.e., *CO, *NO, *OCNO, *NOCONO) during synthesis. Density functional theory calculations revealed promote coadsorption *NO3, as well *OCNO significantly improving kinetics. study underscores critical role facilitating selectivity.

Language: Английский

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A Copper–Zinc Cyanamide Solid-Solution Catalyst with Tailored Surface Electrostatic Potentials Promotes Asymmetric N-Intermediate Adsorption in Nitrite Electroreduction

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: 147(9), P. 8012 - 8023

Published: Feb. 18, 2025

The electrocatalytic nitrite reduction (NO2RR) converts nitrogen-containing pollutants to high-value ammonia (NH3) under ambient conditions. However, its multiple intermediates and multielectron coupled proton transfer process lead low activity NH3 selectivity for the existing electrocatalysts. Herein, we synthesize a solid-solution copper-zinc cyanamide (Cu0.8Zn0.2NCN) with localized structure distortion tailored surface electrostatic potential, allowing asymmetric binding of NO2-. It exhibits outstanding NO2RR performance Faradaic efficiency ∼100% an yield 22 mg h-1 cm-2, among best such process. Theoretical calculations in situ spectroscopic measurements demonstrate that Cu-Zn sites coordinated linear polarized [NCN]2- could transform symmetric [Cu-O-N-O-Cu] CuNCN-NO2- [Cu-N-O-Zn] configuration Cu0.8Zn0.2NCN-NO2-, thus enhancing adsorption bond cleavage. A paired electro-refinery Cu0.8Zn0.2NCN cathode reaches 2000 mA cm-2 at 2.36 V remains fully operational industrial-level 400 >140 h production rate ∼30 mgNH3 cm-2. Our work opens new avenue tailoring potentials using strategy advanced electrocatalysis.

Language: Английский

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Subnanometric Nickel Phosphide Heteroclusters with Highly Active Ni^δ+–P^δ− Pairs for Nitrate Reduction toward Ammonia

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

Published: March 26, 2025

The development of efficient electrocatalysts for the neutral nitrate reduction reaction (NO3–RR) toward ammonia (NH3) is essential to address environmental issues caused by NO3– but remains considerably challenging owing sluggish kinetics NO3–RR in media. Herein, we report subnanometric heteroclusters with strongly coupled nickel–phosphorus (Ni–P) dual-active sites as boost NO3–RR. Experimental and theoretical results reveal that feature Ni–P promotes electron transfer from Ni P, generating Niδ+–Pδ− active pairs, which Niδ+ species are highly Pδ− tunes interfacial water hydrogen bonding network promote dissociation step accelerate proton during Consequently, NO3–RR, exhibit a large NH3 yield rate 0.61 mmol h–1 cm–2 at −0.8 V versus reversible electrode, 2.8- 3.3-fold larger than those on nanoparticles clusters, respectively, generated exists NH4+ electrolytes. This study offers an approach boosting electrocatalytic reactions multiple intermediates designing sites.

Language: Английский

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Co-engineering of Fe-Mn nanocluster with porous carbon for enhanced electrocatalytic ammonia synthesis

Chemical Communications, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Here, we developed iron–manganese nanocluster oxide-loaded nitrogen/oxygen-doped porous carbon towards effective NO 3 RR and Zn–nitrate batteries.

Language: Английский

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Coupling Anodic Reactions in Electrochemical Nitrate Reduction to Ammonia

ChemElectroChem, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 28, 2025

Abstract Ammonia is a widely produced chemical globally, primarily used in fertilizers and products. Recently, it has gained attention as green hydrogen carrier due to its high content energy density. However, the conventional Haber‐Bosch process for ammonia synthesis energy‐intensive, requiring temperatures pressures. Also, significant source of CO 2 emissions. To address these environmental concerns, electrochemical nitrate reduction reaction (NO 3 RR) emerged promising approach production, utilizing from wastewater renewable sources. While most previous research focuses on cathodic needs emphasize importance optimizing anodic reactions NO RR systems reduce consumption improve efficiency. The oxygen evolution (OER), typically coupled with RR, kinetically slow requires standard potential. Therefore, alternative lower potentials not only save but also yield valuable byproducts. Furthermore, coupling like zinc oxidation allows power generation, where positive cell potential indicates spontaneous reactions. This dual approach, saving opens new pathways sustainable reducing overall demands while supporting shift toward systems.

Language: Английский

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High-entropy FeCoNiCuRu solid solutions triggered cocktail effect to achieve fine-tuning adsorption energy for boosting nitrate electroreduction to ammonia

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 500, P. 157426 - 157426

Published: Nov. 1, 2024

Language: Английский

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Solar-Driven High-Rate Ammonia Production from Wastewater Coupled with Plastic Waste Reforming

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 28, 2025

Solar-powered electrochemical NH3 synthesis offers the benefits of sustainability and absence CO2 emissions but suffers from a poor solar-to-ammonia yield rate (SAY) due to low selectivity, large bias caused by sluggish oxygen evolution reaction, photocurrent in corresponding photovoltaics. Herein, highly efficient photovoltaic-electrocatalytic system enabling high-rate solar-driven was developed. A high-performance Ru-doped Co nanotube catalyst used selectively promote nitrite reduction reaction (NO2RR), exhibiting faradaic efficiency 99.6% half-cell energy 52.3% at 0.15 V vs reversible hydrogen electrode, delivering high NO2RR selectivity even electrolytes with NO3- NO2- concentrations. Thus, promoted coupled ethylene glycol oxidation perovskite photovoltaic cell achieve highest SAY reported date (146 ± 1 μmol h-1 cm-2) stable operation.

Language: Английский

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Embedding Pure‐Phase Fe₃C Functional Sites Into Biochar Matrix for Multi‐Scenario Electrocatalytic Ammonia Synthesis and Energy Conversion Utilization

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

Published: Feb. 7, 2025

Abstract The rational design and development of application‐oriented advanced functional catalysts is crucial for facilitating the conversion nitrogen oxides into high‐value ammonia. Herein, biomass derived from pomelo peel, which rich in metal complex groups exhibits a metallic foam‐like framework, utilized as precursor. Iron carbide (Fe 3 C) active sites are incorporated locally 2D, globally 3D biochar structure, enabling multi‐scenario green synthesis ammonia integrated energy utilization. As catalyst, Fe C‐BC achieved an yield rate up to 102120.53 µg h⁻¹ mg cat ⁻¹, with maximum selectivity 100%. A flow‐based electrolysis system featuring not only facilitated continuous but also enhanced solar harvesting. Additionally, nitrate battery employing anode exhibited high output enabled self‐driven synthesis, offering novel insights operational solutions future production. Density‐functional‐theory calculations confirmed that C actively reduces barrier key steps eNitRR process while accelerating water dissociation promote sustained proton supply. These findings collectively provide promising foundation advancing ammonia, emphasizing both efficient catalytic performance sustainable integration.

Language: Английский

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