Product Control in Visible-Light-Driven CO₂ Reduction by Switching Metal Centers of Binuclear Catalysts

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 2522 - 2530

Published: Jan. 27, 2025

Language: Английский

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Intricacies of Mass Transport during Electrocatalysis: A Journey through Iron Porphyrin-Catalyzed Oxygen Reduction

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 15619 - 15626

Published: May 23, 2024

Electrochemical steps are increasingly attractive for green chemistry. Understanding reactions at the electrode–solution interface, governed by kinetics and mass transport, is crucial. Traditional insights into these mechanisms limited, but our study bridges this gap through an integrated approach combining voltammetry, electrochemical impedance spectroscopy, electrospray ionization spectrometry. This technique offers real-time monitoring of chemical processes tracking changes in intermediates products during reactions. Applied to reduction oxygen catalyzed iron(II) tetraphenyl porphyrin complex, it successfully reveals various reaction degradation pathways under different kinetic regimes. Our findings illuminate complex electrocatalytic propose new ways studying alternating current voltage-pulse electrosynthesis. advancement enhances capacity optimize more sustainable processes.

Language: Английский

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Synergistic Effect Promotes Visible‐Light–Driven CO₂‐To‐CO Conversion by Macrocyclic Dinuclear Mixed‐Valence Co (II)/Co (III) Complexes

Applied Organometallic Chemistry, Journal Year: 2025, Volume and Issue: 39(2)

Published: Jan. 12, 2025

ABSTRACT The catalytic conversion of carbon dioxide (CO 2 ) into valuable energy under light sources is one the effective ways to achieve cycle. reported nonprecious metal complex catalysts still show shortcomings low activity and selectivity in visible‐light–driven CO reduction, especially aqueous systems. Herein, we report three dinuclear mixed‐valence Co (II)/Co (III) complexes 1 – 3 bearing macrocyclic ligands that exhibit high for photocatalytic reduction an system. Moreover, TON reach as 4100 96%, respectively, which about 4.9 times higher than mononuclear (II) 4 . Through electrochemical DFT calculations, found increase due synergistic effect between two centers, site stabilizes *COOH intermediate reduces barrier rate‐determining step, thereby increasing activity.

Language: Английский

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Co^II-organic ‘soft’ metallo-supramolecular polymer nanofibers for efficient photoreduction of CO₂

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

Published: Jan. 1, 2025

This study investigates the visible light-driven CO 2 reduction to using 'soft' metallo-supramolecular polymer nanofibers, showcasing high selectivity and efficiency in both pure low-concentration (5% , 95% Ar) enviornments.

Language: Английский

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Electrocatalytic CO2 Reduction Coupled with Water Oxidation by bi- and Tetranuclear Copper Complexes Based on di-2-pyridyl Ketone Ligand

Molecules, Journal Year: 2025, Volume and Issue: 30(7), P. 1544 - 1544

Published: March 31, 2025

In the field of sustainable energy conversion and storage technologies, copper-based complexes have become a research hotspot due to their efficient stable catalytic performance. The development bifunctional catalysts that can simplify steps, enhance efficiency, reduce catalyst usage has an important area. this study, we successfully synthesized two copper with different geometries utilizing di(2-pyridyl) ketone as ligand, [CuII2L2Cl2]·0.5H2O (1) [Cu4IIL4(OCH3)2](NO3)2 (2) (L = deprotonated methoxy-di-pyridin-2-yl-methanol), which serve homogeneous electrocatalysts for water oxidation CO2 reduction simultaneously. turnover frequency (TOF) 1 2 electrocatalytic are 7.23 s−1 0.31 under almost neutral condition (pH 8.22), respectively. Meanwhile, TOF CO 4.27 8.9 s−1, addition, both remain essentially unchanged during processes, demonstrating good stability. Structural analysis reveals distinct efficiencies originate from geometric configurations: binuclear structure complex facilitates proton-coupled electron transfer oxidation, whereas tetranuclear architecture enhances activation. Complexes represent first molecular capable catalyzing reduction. findings in work open up new avenues advancement artificial photosynthesis simulation

Language: Английский

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Theoretical study of tandem catalysts based on metal porphyrin-phthalocyanine two-dimensional carbon-rich conjugated frameworks for the co-reduction of NO3− and CO2 in the electrosynthesis of methylamine

Materials Today Communications, Journal Year: 2024, Volume and Issue: 41, P. 110246 - 110246

Published: Aug. 28, 2024

Language: Английский

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Electron effect regulation: A study on the influence of electron-donating and withdrawing group modification on the performance of metal-coordinated catalysts for electrochemical carbon dioxide reduction

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 683, P. 387 - 397

Published: Dec. 14, 2024

Language: Английский

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Constructing a Stable Built-In Electric Field in Bi/Bi₂Te₃ Nanowires for Electrochemical CO₂ Reduction Reaction

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(23), P. 10809 - 10816

Published: May 30, 2024

Electrochemically converting carbon dioxide (CO

Language: Английский

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Synthesis, Characterization, and Reactivity of a Synthetic End-On Cobalt(II) Alkyl Persulfide Complex as a Model Platform for Thiolate Persulfidation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(31), P. 21999 - 22007

Published: July 24, 2024

Persulfides (RSS

Language: Английский

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Low-valent molecular cobalt complexes for CO2 reduction

Advances in catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 181 - 256

Published: Jan. 1, 2024

Language: Английский

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