The interplay between metals and N-heterocyclic carbenes (NHCs) has provided a window of opportunities for the development of novel catalytic strategies within the past few years. The recent successful combination of Brønsted acids with NHCs has added a new dimension to the field of cooperative catalysis, enabling the stereoselective synthesis of functionalized pyrrolidin-2-ones as valuable scaffolds in heterocyclic chemistry. This Commentary will briefly highlight the concept of N-heterocyclic carbene/Brønsted acid cooperative catalysis as a new and powerful methodology in organic chemistry.
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http://dx.doi.org/10.3762/bjoc.8.43 | DOI Listing |
Chemistry
January 2025
National & Kapodistrian University of Athens, Chemistry, Panepistimiopolis, Zografou, 15771, Athens, GREECE.
The prominence of binuclear catalysts underlines the need for the design and development of diverse bifunctional ligand frameworks that exhibit tunable electronic and structural properties. Such strategies enable metal-metal and ligand-metal cooperation towards catalytic applications, improve catalytic activity, and are essential for advancing multi-electron transfers for catalytic application. Hereby, we present the synthesis, crystal structure, and photocatalytic properties of a binuclear Ni(II) complex, [Ni2(1,10-phenanthroline)2(2-sulfidophenolate)2] (1), which crystallizes in the centrosymmetric triclinic system (P-1) showing extensive intra- and inter- non-coordinated interactions.
View Article and Find Full Text PDFNat Chem
January 2025
Institute of Bioengineering, Swiss Federal Institute of Technology (EPFL), Lausanne, Switzerland.
Protein catalysis and allostery require the atomic-level orchestration and motion of residues and ligand, solvent and protein effector molecules. However, the ability to design protein activity through precise protein-solvent cooperative interactions has not yet been demonstrated. Here we report the design of 14 membrane receptors that catalyse G protein nucleotide exchange through diverse engineered allosteric pathways mediated by cooperative networks of intraprotein, protein-ligand and -solvent molecule interactions.
View Article and Find Full Text PDFFront Mol Biosci
January 2025
Department of Microbiology, Immunology, and Molecular Genetics, University of Kentucky, Lexington, KY, United States.
This study investigates the dynamics of oleate hydratase (OhyA), a bacterial flavoenzyme from , and its interactions with lipid membranes, focusing on the factors influencing membrane binding and oligomerization. OhyA catalyzes the hydration of unsaturated fatty acids, playing a key role in bacterial pathogenesis by neutralizing host antimicrobial fatty acids. OhyA binds the membrane bilayer to access membrane-embedded substrates for catalysis, and structural studies have revealed that OhyA forms oligomers on membrane surfaces, stabilized by both protein-protein and protein-lipid interactions.
View Article and Find Full Text PDFPhilos Trans R Soc Lond B Biol Sci
January 2025
Department of Medicine and Surgery, University of Perugia, P.le L. Severi 1, Perugia 06132, Italy.
Circadian clocks are biological oscillators that evolved to coordinate rhythms in behaviour and physiology around the 24-hour day. In mammalian tissues, circadian rhythms and metabolism are highly intertwined. The clock machinery controls rhythmic levels of circulating hormones and metabolites, as well as rate-limiting enzymes catalysing biosynthesis or degradation of macromolecules in metabolic tissues, such control being exerted both at the transcriptional and post-transcriptional level.
View Article and Find Full Text PDFProtein Sci
February 2025
Center for Cooperative Research in Biomaterials (CIC biomaGUNE), Basque Research and Technology Alliance (BRTA), San Sebastián, Spain.
Enzyme immobilization is indispensable for enhancing enzyme performance in various industrial applications. Typically, enzymes require specific spatial arrangements for optimal functionality, underscoring the importance of correct orientation. Despite well-known N- or C-terminus tailoring techniques, alternatives for achieving orientation control are limited.
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