Assessing the Activity of Transition Metal Oxides for the Electrochemical N₂ Oxidation to Nitrate

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 6315 - 6333

Published: April 3, 2025

Language: Английский

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Chemometrics-boosted protocols for effortless evaluation of factors affecting the electrochemical nitrate reduction to ammonia

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

Published: April 1, 2025

Language: Английский

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Mechanical and Covalent Tailoring of Copper Catenanes for Selective Aqueous Nitrate-to-Ammonia Electrocatalysis

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

Published: April 22, 2025

Electrocatalytic nitrate reduction reaction (NO3RR) for the selective generation of ammonia (NH3) enables removal deleterious pollutants while simultaneously upcycling them into a value-added fertilizer. The development nonprecious metal-derived catalysts such as those featuring copper (Cu) earth-abundant alternatives state-of-the-art precious metal is urgent need yet suffering from activity-selectivity-durability trilemma. Rational design molecular Cu complexes with well-defined coordination structures permitting systematic structure-activity relationship (SAR) investigations key to addressing challenge. Here, series Cu(I) [2]catenane ligands are developed NO3RR electrocatalysts first time. By engineering multiple cationic ammoniums on catenane backbone, acceptance anionic substrate well release ammonium product promoted, thereby facilitating higher Faradaic efficiency and selectivity toward via an 8e- pathway. Of note, mutual Coulombic repulsion between multiply charged overcome by mechanical interlocking that catalyst integrity can be maintained under practical conditions. This report highlights promise employing mechanically interlocked platform customizing redox processes involving proton-coupled electron transfer steps.

Language: Английский

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Challenges and Breakthroughs in Single-Atom Catalysts for Electrocatalytic Nitrate Reduction to Ammonia

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Language: Английский

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Spontaneous Oxidation of Organic Matter and Ammonium Uptake from Manure Wastewater by Redox-Active Materials

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(9), P. 4673 - 4681

Published: Sept. 3, 2024

Spontaneous NH4+ uptake using solid-state redox-active materials, driven by the oxidation of organic matter in manure wastewater, provides a sustainable and energy-friendly method for nutrient recovery. However, mechanisms electron transfer accompanying ion transport are poorly understood. Here, we investigated pathway mechanism analyzing composition changes wastewater via NMR corresponding electrochemical results. We found that spontaneous involves direct process without redox mediators, with co-occurrence intercalation adsorption. Based on elucidated mechanisms, core–shell Prussian blue analogue material improved stability enhanced recovery compared to previously reported electrode materials was developed. Such fundamental understanding compounds can guide design effective resource environmental applications.

Language: Английский

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Design Criteria for Active and Selective Catalysts in the Nitrogen Oxidation Reaction

ACS Physical Chemistry Au, Journal Year: 2024, Volume and Issue: 5(1), P. 38 - 46

Published: Dec. 24, 2024

The direct conversion of dinitrogen to nitrate is a dream reaction combine the Haber–Bosch and Ostwald processes as well steam reforming using electrochemistry in single process. Regrettably, corresponding nitrogen oxidation (NOR) hampered by selectivity problem, since oxygen evolution (OER) both thermodynamically kinetically favored same potential range. This opens search for identification active selective NOR catalysts enable production under anodic conditions. While theoretical considerations computational hydrogen electrode approach have helped identifying material motifs electrocatalytic reactions over last decades, inherent complexity NOR, which consists ten proton-coupled electron transfer steps thus at least nine intermediate states, poses challenge electronic structure theory calculations realm materials screening. To this end, we present different strategy capture competing OER atomic scale. Using data-driven method, provide framework derive generalized design criteria with toward NOR. leads significant reduction costs, only two free-energy changes need be evaluated draw first conclusion on selectivity.

Language: Английский

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Concentrating Nitrogen Waste with Electrodialysis for Fertilizer Production

Environmental Science & Technology Letters, Journal Year: 2024, Volume and Issue: 11(12), P. 1413 - 1419

Published: Nov. 5, 2024

Recovery of nitrogen from wastewater presents a unique opportunity to valorize waste and contribute more circular economy. However, dilute solution separations are challenging for most state-of-the-art technologies. This often results in technologies having low concentration factors that result low-value products (e.g., < 1 wt % N). Here, we demonstrate how cascading electrodialysis system combined with hollow fiber membrane contactor (ED+HFMC) can achieve efficient recovery ammonia simulated centralized animal feeding operation (CAFO) wastewater. The integrated achieved an overall factor ∼200× (∼40× ED ∼5× HFMC). resulted ∼10 NH

Language: Английский

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