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Université de Fribourg

Correlation of MLCTs of Group 7 fac-[M(CO)3]+ complexes (M = Mn, Re) with bipyridine, pyridinylpyrazine, azopyridine, and pyridin-2-ylmethanimine type ligands for rational photoCORM design

Kottelat, Emmanuel ; Lucarini, Fiorella ; Crochet, Aurelien ; Ruggi, Albert ; Zobi, Fabio

In: European Journal of Inorganic Chemistry, 2019, vol. 2019, no. 33, p. 3758–3768

A mathematical correlation of the MLCT absorption maxima of structurally related fac‐ [M(CO)3L2Br] complexes (M = Mn, Re; L2 = bidentate ligand) is obtained by the comparison of a total of 50 species bearing bipyridine, pyridinylpyrazine, azopyridine and pyridin‐2‐ylmethanimine L2 type ligands. The empirical relationship is first derived by the initial comparison of the MLCT absorption...

Université de Fribourg

Tautomerism as primary signaling mechanism in metal sensing: the case of amide group

Deneva, Vera ; Dobrikov, Georgi ; Crochet, Aurelien ; Nedeltcheva, Daniela ; Fromm, Katharina M. ; Antonov, Liudmil

In: Beilstein Journal of Organic Chemistry, 2019, vol. 15, no. 1, p. 1898–1906

The concept for sensing systems using the tautomerism as elementary signaling process has been further developed by synthesizing a ligand containing 4- (phenyldiazenyl)naphthalene-1-ol as a tautomeric block and an amide group as metal capturing antenna. Although it has been expected that the intramolecular hydrogen bonding (between the tautomeric hydroxy group and the nitrogen atom from the...

Université de Fribourg

Isomerization and aggregation of 2-(2-(2-hydroxy-4-nitrophenyl)hydrazono)-1-phenylbutane-1,3-dione: Recent evidences from theory and experiment

Hristova, Silvia ; Kamounah, Fadhil S. ; Crochet, Aurelien ; Hansen, Poul Erik ; Fromm, Katharina M. ; Nedeltcheva, Daniela ; Antonov, Liudmil

In: Journal of Molecular Liquids, 2019, vol. 283, p. 242–248

The title compound potentially can exist as four isomers in solution. Recently Lycka has proposed a protocol for distinguishing two of them based on 15N NMR. This approach has been confirmed theoretically, in the current study, and further developed into a logical scheme that allows the existence of each of the isomers to be proven in solution. The experimental data, obtained by NMR and...

Université de Fribourg

Versatile synthesis of chiral 6-oxoverdazyl radical ligands – new building blocks for multifunctional molecule-based magnets

Solea, Atena B. ; Wohlhauser, Tobie ; Abbasi, Parisa ; Mongbanziama, Yvan ; Crochet, Aurelien ; Fromm, Katharina M. ; Novitchi, Ghenadie ; Train, Cyrille ; Pilkington, Melanie ; Mamula, Olimpia

In: Dalton Transactions, 2018, vol. 47, no. 14, p. 4785–4789

A versatile synthetic methodology to access the first family of chiral verdazyl N,N′- chelate ligands is described and exemplified by N,N′-dimethyl-, N,N′-di-isopropyl- and N,N′-diphenyl oxoverdazyls bearing two isomers of the pinene-pyridine functional group. Their physical properties were probed by X-band EPR spectroscopy, cyclic voltammetry and DFT calculations. Preliminary...

Université de Fribourg

Heptacoordinate Coii complex: a new architecture for photochemical hydrogen production

Lucarini, Fiorella ; Pastore, Mariachiara ; Vasylevskyi, Serhii ; Varisco, Massimo ; Solari, Euro ; Crochet, Aurelien ; Fromm, Katharina M. ; Zobi, Fabio ; Ruggi, Albert

In: Chemistry - A European Journal, 2017, p. -

The first heptacoordinate cobalt catalyst for light-driven hydrogen production in water has been synthesized and characterized. Photochemical experiments using [Ru(bpy)₃]²⁺ as photosensitizer gave a turnover number (TON) of 16300 mol H₂ (mol cat.)⁻¹ achieved in 2 hours of irradiation with visible (475 nm) light. This promising result provides a path forward in the...

Université de Fribourg

Tandem ring‐opening–ring‐closing metathesis for functional metathesis catalysts

Nagarkar, Amit A. ; Yasir, Mohammad ; Crochet, Aurelien ; Fromm, Katharina M. ; Kilbinger, Andreas F. M.

In: Angewandte Chemie International Edition, 2016, vol. 55, no. 40, p. 12343–12346

Use of a tandem ring-opening–ring-closing metathesis (RORCM) strategy for the synthesis of functional metathesis catalysts is reported. Ring opening of 7-substituted norbornenes and subsequent ring-closing metathesis forming a thermodynamically stable 6-membered ring lead to a very efficient synthesis of new catalysts from commercially available Grubbs’ catalysts. Hydroxy functionalized...

Université de Fribourg

The first phospho­ramide-mercury(II) complex with a Cl₂Hg-OP[N(C)(C)]₃ segment

Saneei, Anahid ; Pourayoubi, Mehrdad ; Crochet, Aurelien ; Fromm, Katharina M.

In: Acta Crystallographica C, 2016, vol. 72, p. 230-233

Mercury(II) exhibits a strong preference for linear coordination which has been attributed to relativistic effects splitting the 6p orbitals and promoting sp hybridization. If the two ligands attached to the mercury(II) ion are weak donors, the metal ion can act as a good Lewis acid and expand its coordination number. Moreover, mercury has a special affinity for softer bases,...

Université de Fribourg

Controlled tautomeric switching in azonaphthols tuned by substituents on the phenyl ring

Antonov, Liudmil ; Deneva, Vera ; Simeonov, Svilen ; Kurteva, Vanya ; Crochet, Aurelien ; Fromm, Katharina M. ; Shivachev, Boris ; Nikolova, Rositsa ; Savarese, Marika ; Adamo, Carlo

In: ChemPhysChem, 2015, vol. 16, no. 3, p. 649–657

A series of new tautomeric azonaphthols are synthesized and the possibilities for molecular switching are investigated using molecular spectroscopy, X-ray analysis and density functional theory quantum chemical calculations. Two opposite effects that influence switching are studied: attaching a piperidine sidearm, and adding substituents to the phenyl ring. On the one hand, the attached...

Université de Fribourg

Cis-Dioxido-molybdenum(VI) complexes of tridentate ONO hydrazone Schiff base: Synthesis, characterization, X-ray crystal structure, DFT calculation and catalytic activity

Ebrahimipour, S. Yousef ; Khabazadeh, , , Hojatollah ; Castro, Jesús ; Sheikhshoaie, Iran ; Crochet, Aurelien ; Fromm, Katharina M.

In: Inorganica Chimica Acta, 2015, vol. 427, p. 52–61

Two new cis-MoO₂ [MoO₂(L)(EtOH)] (1), [MoO₂(L)(Py)] (2) [L: (3-methoxy-2oxidobenzylidene)benzohydrazidato], complexes have been synthesized and fully characterized on the basis of elemental analysis, FT-IR, molar conductivity, ¹H NMR, ¹³C NMR and electronic spectra. The structure of complexes has been accomplished by single crystal X-ray...