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Electrification of a Milstein-type catalyst for alcohol reformation

Tocqueville, Damien ; Crisanti, Francesco ; Guerrero, Julian ; Nubret, Esther ; Robert, Marc ; Milstein, David ; von Wolff, Niklas

Chemical science (Cambridge), 2022-11, Vol.13 (44), p.1322-13224 [Periódico revisado por pares]

Cambridge: Royal Society of Chemistry

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  • Título:
    Electrification of a Milstein-type catalyst for alcohol reformation
  • Autor: Tocqueville, Damien ; Crisanti, Francesco ; Guerrero, Julian ; Nubret, Esther ; Robert, Marc ; Milstein, David ; von Wolff, Niklas
  • Assuntos: Alcohols ; Catalysis ; Catalysts ; Chemical industry ; Chemical Sciences ; Chemistry ; Electrification ; Electrochemical oxidation ; Esters ; Ethanol ; Ethyl acetate ; Industrial development ; Organic chemistry ; Ruthenium
  • É parte de: Chemical science (Cambridge), 2022-11, Vol.13 (44), p.1322-13224
  • Notas: https://doi.org/10.1039/d2sc04533h
    Electronic supplementary information (ESI) available: Including experimental procedures, CV-characterization of key intermediates, CPE results, DFT-calculated redox potentials and BDFEs. See DOI
    ObjectType-Article-1
    SourceType-Scholarly Journals-1
    ObjectType-Feature-2
    content type line 23
    These authors contributed equally.
  • Descrição: Novel energy and atom efficiency processes will be keys to develop the sustainable chemical industry of the future. Electrification could play an important role, by allowing to fine-tune energy input and using the ideal redox agent: the electron. Here we demonstrate that a commercially available Milstein ruthenium catalyst ( 1 ) can be used to promote the electrochemical oxidation of ethanol to ethyl acetate and acetate, thus demonstrating the four electron oxidation under preparative conditions. Cyclic voltammetry and DFT-calculations are used to devise a possible catalytic cycle based on a thermal chemical step generating the key hydride intermediate. Successful electrification of Milstein-type catalysts opens a pathway to use alcohols as a renewable feedstock for the generation of esters and other key building blocks in organic chemistry, thus contributing to increase energy efficiency in organic redox chemistry. Electrification of the Milstein catalyst enabled successful molecular electrocatalytic oxidation of ethanol to the four-electron products acetate and ethyl acetate.
  • Editor: Cambridge: Royal Society of Chemistry
  • Idioma: Inglês
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