Boosted Nitrate and CO₂ Reduction for Urea Electrosynthesis on p-Block Bi Dispersed Ru Alloys

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

Published: Feb. 10, 2025

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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Boosting Synergistic Catalysis C–N Coupling via Stabilizing Close Zn/Ti Bimetallic Sites for Electrocatalytic Urea Synthesis from CO₂ and Nitrite

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 2703 - 2714

Published: Jan. 30, 2025

Electrocatalytic urea synthesis is significantly limited by the low efficiency of C–N bond coupling between CO2 and nitrite. Here, we designed a Zn Ti bimetallic active site catalyst anchoring TiO2 on surface ZnO developed new NF@CoMn2O4@ZnO-TiO2 electrocatalyst with high resistance to deactivation. The Co3+/Mn3+-Mn4+ solid oxide pairs in maintain their stability extracting accumulated electrons around Zn2+ Ti4+ through strong electronic interactions. sites can efficiently catalyze reduction *CO, while NO2– *NH2 intermediate product. proximity shortens distance *CO intermediates, facilitating efficient electrocatalytic urea. DFT calculations indicate that ΔG required for adsorbed short-range CoMn2O4@ZnO-TiO2 lower compared CoMn2O4@ZnO ZnO. This results remarkably Faradaic 61.18% at −0.6 V vs RHE NF@CoMn2O4@ZnO-TiO2. work provides pathway achieving synergistic catalysis reactions different metal catalytic sites.

Language: Английский

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Nanoconfinement and tandem catalysis over yolk-shell catalysts towards electrochemical reduction of CO2 to multi-carbon products

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 687, P. 733 - 741

Published: Feb. 15, 2025

Language: Английский

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Electrosynthesis of Urea on High‐Density Ga─Y Dual‐Atom Catalyst via Cross‐Tuning

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

Published: Feb. 25, 2025

Abstract Electrochemically converting carbon dioxide (CO 2 ) and nitrate (NO 3 − into urea via the C─N coupling route offers a sustainable alternative to traditional industrial production technology, but it is still limited by poor yield rate, low Faradaic efficiency, insufficient kinetics. Herein, high‐density Ga─Y dual‐atom catalyst developed with loading up 14.1 wt.% of Ga Y supported on N, P‐co‐doped substrate (Ga/Y‐CNP) for electrosynthesis. The facilitates efficient through co‐reduction CO NO , resulting in high rate 41.9 mmol h −1 g efficiency 22.1% at −1.4 V versus reversible hydrogen electrode. In situ spectroscopy theoretical calculations reveal that superior performance attributed cross‐tuning between adjacent pair sites, which can mutually optimize their electronic states facilitating reduction *CO sites promoting conversion hydroxylamine (*NH OH) followed spontaneous *NH OH intermediates form bonds. This work pioneering strategy manipulate pathways active produce high‐value‐added chemicals.

Language: Английский

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Efficient urea synthesis by coupling catalyst of nickel-single-atom and copper-cluster

Journal of Material Science and Technology, Journal Year: 2025, Volume and Issue: unknown

Published: March 1, 2025

Language: Английский

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