Philipp Gotico, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
Abstract The mass scale catalytic transformation of carbon dioxide (CO 2 ) into reduced forms of carbon is an imperative to address the ever‐increasing anthropogenic emission. Understanding the mechanistic routes leading to the multi‐electron‐proton conversion of CO 2 provides handles for chemists to overcome the kinetically and thermodynamically hard challenges and further optimize these processes. Through extensive electrochemical investigations, Prof. J.‐M. Savéant and coworkers have made invaluable ...
Tópico(s): Carbon dioxide utilization in catalysis
2021 - Wiley | ChemElectroChem
Yabo Wang, Xuepeng Zhang, Haitao Lei, Kai Guo, Gelun Xu, Lisi Xie, Xialiang Li, Wei Zhang, Ulf‐Peter Apfel, Rui Cao,
... to-Ethanol Conversion via Enriched Intermediates at Molecule-Metal Catalyst Interfaces.Nat. Catal.2020, 3, 75–82. Google Scholar 34. Azcarate I.; Costentin C.; Robert M.; Savéant J.-M.Through-Space Charge Interaction Substituent Effects in Molecular Catalysis Leading to the Design of the Most Efficient Catalyst of CO2-to-CO Electrochemical Conversion.J. Am. Chem. Soc.2016, 138, 16639–16644. Google Scholar 35. Gotico P.; Roupnel L.; Guillot R.; Sircoglou M.; Leibl ...
Tópico(s): Electrocatalysts for Energy Conversion
2022 - Chinese Chemical Society | CCS Chemistry
Philipp Gotico, Bernard Boitrel, Régis Guillot, Marie Sircoglou, Annamaria Quaranta, Zakaria Halime, Winfried Leibl, Ally Aukauloo,
Abstract Inspired by nature's orchestra of chemical subtleties to activate and reduce CO 2 , we have developed a family of iron porphyrin derivatives in to which we have introduced urea groups functioning as multipoint hydrogen‐bonding pillars on the periphery of the porphyrinic ring. This structure closely resembles the hydrogen‐bond stabilization scheme of the carbon dioxide (CO 2 ) adduct in the carbon monoxide dehydrogenase (CODH). We found that such changes to the second coordination sphere significantly ...
Tópico(s):
2019 - Wiley | Angewandte Chemie International Edition
Yu Wang, Ning‐Yu Huang, Haoyu Wang, Xuewen Zhang, Jia‐Run Huang, Pei‐Qin Liao, Xiao‐Ming Chen, Jie‐Peng Zhang,
... Ed.2018, 57, 9684–9688. Google Scholar 11. Gotico P.; Boitrel B.; Guillot R.; Sircoglou M.; Quaranta ...
Tópico(s): Electrocatalysts for Energy Conversion
2022 - Chinese Chemical Society | CCS Chemistry
Chanjuan Zhang, Philipp Gotico, Régis Guillot, Diana Dragoé, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
... of carbon monoxide dehydrogenase (CODH) active site two metal ions together with hydrogen bonding scheme from amino ... centers was replaced by a redox inactive Zn metal, questioning the cooperative action of the two metals. Snapshots of X-ray structures indicate that the ...
Tópico(s): Metalloenzymes and iron-sulfur proteins
2022 - Wiley | Angewandte Chemie International Edition
Philipp Gotico, Zakaria Halime, Winfried Leibl, Ally Aukauloo,
... which relies on the synergistic interaction between two metal centers to activate and convert the CO2 substrate. ... can help understand the synergistic effect of two metal centers.
Tópico(s): Cyclopropane Reaction Mechanisms
2023 - Wiley | ChemPlusChem
Philipp Gotico, Bernard Boitrel, Régis Guillot, Marie Sircoglou, Annamaria Quaranta, Zakaria Halime, Winfried Leibl, Ally Aukauloo,
Abstract Inspired by nature's orchestra of chemical subtleties to activate and reduce CO 2 , we have developed a family of iron porphyrin derivatives in to which we have introduced urea groups functioning as multipoint hydrogen‐bonding pillars on the periphery of the porphyrinic ring. This structure closely resembles the hydrogen‐bond stabilization scheme of the carbon dioxide (CO 2 ) adduct in the carbon monoxide dehydrogenase (CODH). We found that such changes to the second coordination sphere significantly ...
Tópico(s):
2019 - Wiley | Angewandte Chemie
Khadija Talbi, Francesc Penas-Hidalgo, Amanda Robinson, Philipp Gotico, Winfried Leibl, Pierre Mialane, María Gómez-Mingot, Marc Fontecave, Albert Solé‐Daura, Caroline Mellot‐Draznieks, Anne Dolbecq,
The photocatalytic activity for CO2 reduction of a series of Ni-substituted polyoxometalates (POMs) differing in nuclearity, shape and size, has been investigated under visible light irradiation, with [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) as photosensitizer and triethanolamine as sacrificial donor. The tetrabutylammonium salt of the Ni4 tetranuclear species was found to exhibit the highest CO production and its stability under photocatalytic conditions was demonstrated. The catalytic performance was significantly ...
Tópico(s):
2024 - Elsevier BV | Applied Catalysis B Environment and Energy
Philipp Gotico, Loïc Roupnel, Régis Guillot, Marie Sircoglou, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
Abstract The manipulation of the second coordination sphere for improving the electrocatalytic CO 2 reduction has led to breakthroughs with hydrogen bonding, local proton source, or electrostatic effects. We have developed two atropisomers of an iron porphyrin complex with two urea functions acting as multiple hydrogen‐bonding tweezers to lock the metal‐bound CO 2 in a similar fashion found in the carbon monoxide dehydrogenase (CODH) enzyme. The αα topological isomer with the two urea groups on the ...
Tópico(s): Carbon dioxide utilization in catalysis
2020 - Wiley | Angewandte Chemie
Philipp Gotico, Loïc Roupnel, Régis Guillot, Marie Sircoglou, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
Abstract The manipulation of the second coordination sphere for improving the electrocatalytic CO 2 reduction has led to breakthroughs with hydrogen bonding, local proton source, or electrostatic effects. We have developed two atropisomers of an iron porphyrin complex with two urea functions acting as multiple hydrogen‐bonding tweezers to lock the metal‐bound CO 2 in a similar fashion found in the carbon monoxide dehydrogenase (CODH) enzyme. The αα topological isomer with the two urea groups on the ...
Tópico(s):
2020 - Wiley | Angewandte Chemie International Edition
Philipp Gotico, Dooshaye Moonshiram, Cunming Liu, Xiaoyi Zhang, Régis Guillot, Annamaria Quaranta, Zakaria Halime, Winfried Leibl, Ally Aukauloo,
Inspired by the sulfur-rich environment found in active hydrogenase enzymes, a Ni-based proton reduction catalyst with pentadentate N2 S3 ligand was synthesised. When coupled with [Ru(bpy)3 ]2+ (bpy=2,2'-bipyridine) as photosensitiser and ascorbate as electron donor in a 1:1 mixture of dimethylacetamide and aqueous ascorbic acid/ascorbate buffer, the catalyst showed improved photocatalytic activity compared with a homologous counterpart bearing a tetradentate N2 S2 ligand. The mechanistic pathway of ...
Tópico(s): Advanced battery technologies research
2019 - Wiley | Chemistry - A European Journal
Iulia Cocosila, Albert Solé‐Daura, Philipp Gotico, Jérémy Forté, Yun Li, Marc Fontecave,
... molecular catalysts and inorganic photosensitizers based on nonnoble metals. The photoreduction of CO2 catalyzed by a series of 11 metal-salophen complexes, based on variously functionalized salophen ligands, ...
Tópico(s):
2024 - American Chemical Society | ACS Catalysis
Philipp Gotico, Christian Herrero, Stefano Protti, Annamaria Quaranta, Sujitraj Sheth, Reza Fallahpour, Rajaa Farran, Zakaria Halime, Marie Sircoglou, Ally Aukauloo, Winfried Leibl,
Electron relays play a crucial role for efficient light-induced activation by a photo-redox moiety of catalysts for multi-electronic transformations. Their insertion between the two units reduces detrimental energy transfer quenching while establishing at the same time unidirectional electron flow. This rectifying function allows charge accumulation necessary for catalysis. Mapping these events in photophysical studies is an important step towards the development of efficient molecular photocatalysts. ...
Tópico(s): Radical Photochemical Reactions
2022 - Springer Science+Business Media | Photochemical & Photobiological Sciences
Eva Pugliese, Nhat Tam Vo, Alain Boussac, Frédéric Banse, Yasmina Mekmouche, A. Jalila Simaan, Thierry Tron, Philipp Gotico, Marie Sircoglou, Zakaria Halime, Winfried Leibl, Ally Aukauloo,
Coupling a photoredox module and a bio-inspired non-heme model to activate O2 for the oxygen atom transfer (OAT) reaction requires a vigorous investigation to shed light on the multiple competing electron transfer steps, charge accumulation and annihilation processes, and the activation of O2 at the catalytic unit. We found that the efficient oxidative quenching mechanism between a [Ru(bpy)3]2+ chromophore and a reversible electron mediator, methyl viologen (MV2+), to form the reducing species methyl ...
Tópico(s): Electrocatalysts for Energy Conversion
2022 - Royal Society of Chemistry | Chemical Science
Adrien Smith, Philipp Gotico, Régis Guillot, Stéphane Le Gac, Winfried Leibl, Ally Aukauloo, Bernard Boitrel, Marie Sircoglou, Zakaria Halime,
... integrate a well-organized pocket around the active metal center. Within this cavity, second coordination sphere functionalities ...
Tópico(s): Advanced battery technologies research
2025 - Wiley | Advanced Science
Chanjuan Zhang, Philipp Gotico, Régis Guillot, Diana Dragoé, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
... their Communication (e202214665). The cooperativity between the two metal centres of the catalyst was shown for both ...
Tópico(s): Asymmetric Hydrogenation and Catalysis
2023 - Wiley | Angewandte Chemie
Chanjuan Zhang, Philipp Gotico, Régis Guillot, Diana Dragoé, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
... their Communication (e202214665). The cooperativity between the two metal centres of the catalyst was shown for both ...
Tópico(s): Electrocatalysts for Energy Conversion
2023 - Wiley | Angewandte Chemie International Edition
Daniel H. Cruz Neto, Eva Pugliese, Philipp Gotico, Annamaria Quaranta, Winfried Leibl, Karine Steenkeste, Daniel Peláez, Thomas Pino, Zakaria Halime, Minh‐Huong Ha‐Thi,
Abstract The development of functional artificial photosynthetic devices relies on the understanding of mechanistic aspects involved in specialized photocatalysts. Modified iron porphyrins have long been explored as efficient catalysts for the light‐induced reduction of carbon dioxide (CO 2 ) towards solar fuels. In spite of the advancements in homogeneous catalysis, the development of the next generation of catalysts requires a complete understanding of the fundamental photoinduced processes taking ...
Tópico(s):
2024 - Wiley | Angewandte Chemie
Eva Pugliese, Philipp Gotico, Iris Wehrung, Bernard Boitrel, Annamaria Quaranta, Minh‐Huong Ha‐Thi, Thomas Pino, Marie Sircoglou, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
Die Entschlüsselung des Mechanismus der Ladungsakkumulation bei der lichtgetriebenen Kohlendioxidreduktion unter Verwendung von wasserstoffverbrückten Eisenporphyrinen liefert neue Einblicke in den geschwindigkeitsbegrenzenden Schritt. Während der formale Fe(0)-Redoxzustand weithin als die katalytisch aktive Spezies galt, zeigen Zakaria Halime, Ally Aukauloo et al. in ihrer Zuschrift (DOI: 10.1002/ange.202117530), dass die Fe(I)-Spezies bereits an der Substrataktivierung des photokatalytischen Zyklus ...
Tópico(s):
2022 - Wiley | Angewandte Chemie
Chanjuan Zhang, Philipp Gotico, Régis Guillot, Diana Dragoé, Winfried Leibl, Zakaria Halime, Ally Aukauloo,
Abstract At the core of carbon monoxide dehydrogenase (CODH) active site two metal ions together with hydrogen bonding scheme from amino acids orchestrate the interconversion between CO 2 and CO. We have designed a molecular catalyst implementing a bimetallic iron complex with an embarked second coordination sphere with multi‐point hydrogen‐bonding interactions. We found that, when immobilized on carbon paper electrode, the dinuclear catalyst enhances up to four fold the heterogeneous CO 2 reduction ...
Tópico(s): Metalloenzymes and iron-sulfur proteins
2022 - Wiley | Angewandte Chemie