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| Naji, M. |
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| Motta, Antonella |
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| Aletan, Dirar |
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| Mohamed, Tarek |
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| Ertürk, Emre |
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| Azam, Siraj |
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| Rančić, M. |
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| Ollier, Nadège |
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| Azevedo, Nuno Monteiro |
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| Landes, Michael |
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Mazzaro, Raffaello
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Publications (5/5 displayed)
- 2023An advanced PdNPs@MoS<sub>2</sub> nanocomposite for efficient oxygen evolution reaction in alkaline mediacitations
- 2023Photoelectrochemical Valorization of Biomass Derivatives with Hematite Photoanodes Modified by Cocatalystscitations
- 2023Robust Molecular Anodes for Electrocatalytic Water Oxidation Based on Electropolymerized Molecular Cu Complexescitations
- 2022NiCo2O4 nanostructures loaded onto pencil graphite rod: An advanced composite material for oxygen evolution reactioncitations
- 2022NiNP@rGO Nanocomposites as Heterogeneous Catalysts for Thiocarboxylation Cross-Coupling Reactionscitations
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article
Robust Molecular Anodes for Electrocatalytic Water Oxidation Based on Electropolymerized Molecular Cu Complexes
Abstract
<jats:title>Abstract</jats:title><jats:p>A multistep synthesis of a new tetra‐amidate macrocyclic ligand functionalized with alkyl‐thiophene moieties, 15,15‐bis(6‐(thiophen‐3‐yl)hexyl)‐8,13‐dihydro‐5H‐dibenzo[b,h][1,4,7,10]tetraazacyclotridecine‐6,7,14,16(15H,17H)‐tetraone, H<jats:sub>4</jats:sub><jats:bold>L</jats:bold>, is reported. The reaction of the deprotonated ligand, <jats:bold>L</jats:bold><jats:sup>4−</jats:sup>, and Cu(II) generates the complex [<jats:bold>LCu</jats:bold>]<jats:sup>2−</jats:sup>, that can be further oxidized to Cu(III) with iodine to generate [<jats:bold>LCu</jats:bold>]<jats:sup>−</jats:sup>. The H<jats:sub>4</jats:sub><jats:bold>L</jats:bold> ligand and their Cu complexes have been thoroughly characterized by analytic and spectroscopic techniques (including X‐ray Absorption Spectroscopy, XAS). Under oxidative conditions, the thiophene group of [<jats:bold>LCu</jats:bold>]<jats:sup>2‐</jats:sup> complex polymerizes on the surface of graphitic electrodes (glassy carbon disks (<jats:bold>GC</jats:bold>), glassy carbon plates (<jats:bold>GC<jats:sub>p</jats:sub></jats:bold>), carbon nanotubes (<jats:bold>CNT</jats:bold>) or graphite felts (<jats:bold>GF</jats:bold>)) generating highly stable thin films. With CNTs deposited on a GC by drop casting, we obtain hybrid molecular materials labeled as <jats:bold>GC/CNT@p‐[LCu]<jats:sup>2−</jats:sup></jats:bold>. The latter are characterized by electrochemical techniques that show their capacity to electrocatalytically oxidize water to dioxygen at neutral pH. These new molecular anodes achieve current densities in the range of 0.4 mA/cm<jats:sup>2</jats:sup> at 1.30 V versus NHE with an onset overpotential at approx. 250 mV. Bulk electrolysis experiments show an excellent stability achieving TONs in the range of 7600 during 24 h with no apparent loss of catalytic activity and maintaining the molecular catalyst integrity, as evidenced by electrochemical techniques and XAS spectroscopy. Further with highly porous graphitic materials such as <jats:bold>GF</jats:bold>, we obtain TONs in the range of 11,000.</jats:p><jats:p>This article is protected by copyright. All rights reserved</jats:p>