Palladium‐Based Dyotropic Rearrangement Enables A Triple Functionalization of Gem‐Disubstituted Alkenes: An Unusual Fluorolactonization Reaction

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Carbon Dioxide Reduction by Multimetallic Uranium(IV) Complexes Supported by Redox-Active Schiff Base Ligands

Rosario Scopelliti, Marinella Mazzanti, Marta Falcone, Nadir Jori

The synthesis, structure, and reactivity with CO2 and CS2 of new U(IV) complexes with a redox-active Schiff base are reported. The reaction of UI3 with the heptadentate Schiff base ligand 2,2',2 ''-tris(salicylideneimino)-triethylamine (trensal) did not le ...

2020

Spectroscopic Evidence for Peptide-Bond-Selective Ultraviolet Photodissociation

Oleg Boyarkine, Vladimir Kopysov, Aleksandr Pereverzev

We study the photodissociation induced by ultraviolet excitation of amide bonds in gas-phase protonated peptides. Jointly, mass spectrometry and cold ion spectroscopy provide evidence for a selective non-statistical dissociation of specific peptide bonds i ...

2020

Revealing Single-Bond Anomeric Selectivity in Carbohydrate-Protein Interactions

Oleg Boyarkine, Aleksandr Pereverzev, Ruslan Yamaletdinov, Viktoriia Aladinskaia

The noncovalent binding of proteins to glycans is amazingly selective to the isoforms of carbohydrates, including alpha/beta anomers that coexist in solution. We isolate in the gas phase and study at the atomic level the simplest model system: noncovalent ...

AMER CHEMICAL SOC2020

Copper-Catalyzed Cyanoalkylative Aziridination of N-Sulfonyl Allylamines

Jieping Zhu, Qian Wang, Minh Tu Ha, Weisi Guo

Reaction of N-arylsulfonyl allylamines with alkyl nitriles in the presence of di-tert-butyl peroxide (DTBP) and a catalytic amount of copper salt afforded homologated aziridines in 43-86% yield. A sequence involving addition of the in situ generated cyanom ...

Wiley2020

Multihole water oxidation catalysis on haematite photoanodes revealed by operando spectroelectrochemistry and DFT

Michael Graetzel, Matthew Thomas Mayer

Water oxidation is the key kinetic bottleneck of photoelectrochemical devices for fuel synthesis. Despite advances in the identification of intermediates, elucidating the catalytic mechanism of this multi-redox reaction on metal-oxide photoanodes remains a ...

NATURE PUBLISHING GROUP2020

Cryogenic Infrared Action Spectroscopy Fingerprints the Hydrogen Bonding Network in Gas-Phase Coumarin Cations

Thomas Rizzo, Eduardo Carrascosa Casado, Robert Paul Pellegrinelli

We report cryogenic vibrational spectra of gas-phase cations of two common hydroxycoumarins, scopoletin and esculetin, as well as their glycosidic derivatives, scopolin and esculin. The study allows direct observation of the intramolecular interactions bet ...

2020

Oxygen evolution reaction catalyzed by first-row transition metal oxides: stability and mechanism

Aliki Moysiadou

Water splitting offers the opportunity for storing solar energy and, thus, producing carbon-neutral and renewable solar fuels. The process, known as artificial photosynthesis, is limited by the electrocatalytic conversion of water into molecular oxygen. El ...

EPFL2020

Yield strength and misfit volumes of NiCoCr and implications for short-range-order

William Curtin, Binglun Yin

The face-centered cubic medium-entropy alloy NiCoCr has received considerable attention for its good mechanical properties, uncertain stacking fault energy, etc, some of which have been attributed to chemical short-range order (SRO). Here, we examine the y ...

Nature Research2020

Electrons leave the flatland: out-of-plane charge dynamics in layered materials

Edoardo Martino

The goal of this thesis is to explore the "neglected" third dimension of layered materials, by studying the interlayer charge dynamics through dc conductivity, optical spectroscopy and ab-initio calculations. This project was designed to respond to the gro ...

EPFL2020

Cross-linkable polymer, hydrogel, and method of preparation thereof

Dominique Pioletti, Christophe Moser, Pierre-Etienne Bourban, Peyman Karami, Céline Samira Wyss

The invention relates to a cross-linkable polymer comprising a base polymer comprising functional groups at least some of which have been reacted with a first organic molecule comprising a cross-linkable unit and with a second organic molecule capable of b ...

2020

Controlling Single Molecule Conductance by a Locally Induced Chemical Reaction on Individual Thiophene Units

Klaus Kern, Uta Schlickum, Ivan Pentegov, Verena Katharina Schendel

Among the prerequisites for the progress of single-molecule-based electronic devices are a better understanding of the electronic properties at the individual molecular level and the development of methods to tune the charge transport through molecular jun ...

Wiley-VCH Verlag GmbH2020