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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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Taccardi, Nicola |
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Kononenko, Denys |
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Petrov, R. H. | Madrid |
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Alshaaer, Mazen | Brussels |
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Bih, L. |
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Casati, R. |
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Muller, Hermance |
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Kočí, Jan | Prague |
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Šuljagić, Marija |
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Kalteremidou, Kalliopi-Artemi | Brussels |
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Azam, Siraj |
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Ospanova, Alyiya |
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Blanpain, Bart |
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Ali, M. A. |
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Popa, V. |
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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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Rignanese, Gian-Marco |
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Boscherini, Federico
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (8/8 displayed)
- 2023X‐Ray Nanoanalysis Revealing the Role of Electronically Active Passivation Layers in Perovskite X‐Ray film Detectorscitations
- 2023Robust Molecular Anodes for Electrocatalytic Water Oxidation Based on Electropolymerized Molecular Cu Complexescitations
- 2020Doping Evolution of the Local Electronic and Structural Properties of the Double Perovskite Ba2Na1-xCaxOsO6citations
- 2020Doping Evolution of the Local Electronic and Structural Properties of the Double Perovskite Ba$_{2}$Na$_{1–x}$Ca$_{x}$OsO$_{6}$citations
- 2007Formation and dissolution of D-N complexes in dilute nitridescitations
- 2004Structural characterization of epitaxial Y2O3 on Si (001) and of the Y2O3/Si interfacecitations
- 2004X-ray absorption study at the Mg and O K-edges of ultrathin MgO epilayers on Ag(001)citations
- 2004Nio and Mgo ultrathin films by polarization dependent xascitations
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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>