Abstract Influencing electron distribution within a coordination complex bearing redox-active ligands offers the possibility to foster new reactivities. This redistribution can involve electrons but also protons or more elaborate chemical groups. Often perceived as a liability, chemical…
Abstract Selective chemical modifications of biomolecules are in high demand for the development and implementation of chemical biology strategies. Methods involving radicals have emerged as powerful options yet potentially generate side reactivities when involving harsh reaction conditions. We…
Abstract We report the design and synthesis of ratiometric 19F-ATCUN (Xxx-Zzz-His) peptide probes for the selective and reversible detection of Ni2⁺ and Cu2⁺ by 19F NMR spectroscopy. In contrast to fluorescence-based approaches, 19F NMR enables background-free detection in biological media, due to…
Abstract Cooperative multielectron transfer is central to electron storage strategies and small-molecule activation and involves a thermodynamically favored second electron transfer occurring after the first electron transfer. This is the trademark of molecular systems with inverted redox…
Abstract Selective and strategic modification of redox cofactors offers significant advantages for the design of molecular probes, including high compatibility and affinity. This is particularly relevant in the case of redox cofactors with innate fluorescence properties, such as flavins, and…
Abstract Flavins and their alloxazine isomers are key chemical scaffolds for bioinspired electron transfer strategies. Their properties can be fine-tuned by functional groups, which must be introduced at an early stage of the synthesis as their aromatic ring is inert towards post-functionalization.…
Summary We report the design of a unique bioinspired ligand merging redox-active catechol and flavin-related alloxazine substructures. Upon coordination with a Ni(II) salt, this hybrid ligand forms a trinuclear complex containing three NiII centers and three redox-active ligands. This air-stable…
Abstract Biological systems provide attractive reactivity blueprints for the design of challenging chemical transformations. Emulating the operating mode of natural systems may however not be so easy and direct translation of structural observations does not always afford the anticipated…
Summary Metalloenzymes use earth-abundant non-noble metals to perform high-fidelity transformations in the biological world. To ensure chemical efficiency, metalloenzymes have acquired evolutionary reactivity-enhancing tools. Among these, the entatic state model states that a strongly distorted…
Abstract Copper catalysis finds applications in various synthetic fields by utilizing the ability of copper to sustain mono- and bielectronic elementary steps. Further to the development of well-defined copper complexes with classical ligands such as phosphines and N-heterocyclic carbenes, a new…
Abstract Metalloenzymes use earth-abundant non-noble metals to perform high‐fidelity transformations in the biological world. To ensure chemical efficiency, metalloenzymes have acquired evolutionary reactivity‐enhancing tools. Among these, the entatic state model states that a strong steric…
Abstract Metalloenzymes are nature's own catalysts and offer as such endless inspirational source for the chemists seeking selectivity in transformations. Metalloenzymes involved in oxidoreduction processes have specific subunits dedicated to electron and proton transfer, and these so‐called redox…
Non-noble metal catalysis: Molecular approaches and Reactions, Wiley-VCH, edited by Robertus Klein Gebbink and Marc-Etienne Moret, Utrecht University, The Netherlands. The study and development of new homogeneous catalysts based on first-row metals (Mn, Fe, Co, Ni, and Cu) has grown significantly…
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