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Université de Fribourg

Mono-telechelic polymers by catalytic living ring-opening metathesis polymerization with second-generation Hoveyda–Grubbs catalyst

Liu, Peng ; Dong, Zhenghao ; Kilbinger, Andreas F. M.

In: Materials Chemistry Frontiers, 2020, vol. 4, no. 9, p. 2791–2796

The second-generation Hoveyda–Grubbs (HG2) catalyst, which has a small initiation to propagation rate ratio (ki/kp) in ring-opening metathesis polymerization (ROMP), was successfully used in a recently developed catalytic living ROMP. This proved that slow-initiating catalysts can enable ROMP in a living fashion to produce polymers with narrow dispersity and controlled molecular weight. The...

Université de Fribourg

One-step ring opening metathesis block-like copolymers and their compositional analysis by a novel retardation technique

Yasir, Mohammad ; Liu, Peng ; Markwart, Jens C. ; Suraeva, Oksana ; Wurm, Frederik R. ; Smart, Jansie ; Lattuada, Marco ; Kilbinger, Andreas F. M.

In: Angewandte Chemie International Edition, 2020, vol. 59, no. 32, p. 13597-13601

Using a one-step synthetic route for block copolymers avoids the repeated addition of monomers to the polymerization mixture, which can easily lead to contamination and, therefore, to the unwanted termination of chain growth. For this purpose, monomers (M1–M5) with different steric hindrances and different propagation rates are explored. Copolymerization of M1 (propagating rapidly) with M2...

Université de Fribourg

Understanding the assembly of amphiphilic additives in bulk and dispersed non-lamellar lipid-based matrices: Phosphorylation, H-bonding and ionisation

F.Etter, Marco ; Dellenbach, Daria ; Petri-Fink, Alke ; Rothen-Rutishauser, Barbara ; M.Landau, Ehud ; Fong, Wye-Khay

In: Journal of Colloid and Interface Science, 2020, vol. 562, p. 502–510

The aqueous channel size of lipidic cubic phases can be a limiting factor for certain applications. For this reason, additives have been used to exquisitely control their nanostructure. In this study, two families of primary phosphoesters have been designed, synthesised and utilised to determine the effect of the positioning of the guest additive at the interface of the host mesophase, and to...

Université de Fribourg

Preparation of metallosupramolecular single-chain polymeric nanoparticles and their characterization by Taylor dispersion

Neumann, Laura N. ; Urban, Dominic A. ; Lemal, Philipp ; Ramani, Sushila ; Petri-Fink, Alke ; Balog, Sandor ; Weder, Christoph ; Schrettl, Stephen

In: Polymer Chemistry, 2020, vol. 11, no. 2, p. 586–592

Intramolecular cross-linking of polymers can furnish single-chain polymeric nanoparticles (SCPNs), and the use of reversible non-covalent bonds for cross-linking can potentially provide such nanoparticles with stimuli-responsive properties. Here, we report the synthesis of acrylic polymers that carry pendant 2,6-bis(1′-methyl- benzimidazolyl)pyridine ligands, and use these for the...

Université de Fribourg

Telechelics based on catalytic alternating ring-opening metathesis polymerization

Pal, Subhajit ; Alizadeh, Mahshid ; Kilbinger, Andreas F. M.

In: ACS Macro Letters, 2019, vol. 8, no. 10, p. 1396–1401

We describe a protocol to synthesize alternating telechelic ROMP copolymers of 7- oxa-norbornene derivatives and cycloalkenes under catalytic conditions. These copolymers were synthesized using Grubbs’ second-generation catalyst. The sterically less hindered backbone double bonds of the resulting alternating copolymers facilitate the chain transfer (secondary metathesis) reactions. In the ...

Université de Fribourg

Synthesis and properties of poly(norbornene)s with lateral aramid groups

Kong, Phally ; Drechsler, Susanne ; Balog, Sandor ; Schrettl, Stephen ; Weder, Christoph ; Kilbinger, Andreas F. M.

In: Polymer Chemistry, 2019, vol. 10, no. 16, p. 2057–2063

This paper deals with the synthesis and investigation of comb-like poly(norbornene)s carrying lateral rod-like aramid groups. Two types of norbornene-based monomers were synthesized and copolymerized with a norbornene carrying an aliphatic side chain using ring opening metathesis polymerization (ROMP). The new monomers contain aramid derivatives that display different types of non-covalent...

Université de Fribourg

Functional polymers through mechanochemistry

Schrettl, Stephen ; Balkenendea, Diederik W. R. ; Calvino, Céline ; Karman, Marc ; Lavrenova, Anna ; Neumann, Laura N. ; Sagaraa, Yoshimitsu ; Verde-Sestoa, Ester ; Giannantonio, Michela di ; Simon, Yoan C. ; Fromm, Katharina M. ; Lattuada, Marco ; Weder, Christoph

In: CHIMIA International Journal for Chemistry, 2019, vol. 73, no. 1, p. 7–11

While coupling mechanical and chemical processes is widespread in living organisms, the idea to harness the mechanically induced dissociation of weak covalent and non- covalent bonds to create artificial materials that respond to mechanical stimulation has only recently gained attention. Here we summarize our activities that mainly revolve around the exploitation of non-covalent interactions...

Université de Fribourg

Towards polymers with molecular auxeticity

Alizadeh, Mahshid ; Tennie, Iris K. ; Steiner, Ullrich ; Kilbinger, Andreas F. M.

In: CHIMIA International Journal for Chemistry, 2019, vol. 73, no. 1, p. 25–28

For many decades, it has been challenging to synthesize auxetic materials at the molecular level. Auxetic materials exhibit counterintuitive behavior; they expand perpendicularly to the direction in which they are stretched. An aromatic macrocycle containing a sequence of N-substituted and N-unsubstituted amides was designed to resemble the re-entrant structure found in macromolecular auxetic...

Université de Fribourg

Catalytic living ring-opening metathesis polymerization with Grubbs’ second- and third-generation catalysts

Yasir, Mohammad ; Liu, Peng ; Tennie, Iris K. ; Kilbinger, Andreas F. M.

In: Nature Chemistry, 2019, vol. 11, no. 5, p. 488–494

In a conventional living ring-opening metathesis polymerization (ROMP), an equal number of ruthenium complexes to the number of polymer chains synthesized are required. This can lead to high loadings of ruthenium complexes when aiming for shorter polymers. Here, a reversible chain-transfer agent was used to produce living ROMP polymers from norbornene derivatives using catalytic amounts of...