RT Journal Article
T1 Silver-Catalyzed C-C Bond Formation between Methane and Ethyl Diazoacetate in Supercritical CO2
A1 Caballero Bevia, Ana
A1 Despagnet-Ayoub, Emmanuelle
A1 Díaz Requejo, María Mar
A1 Díaz Rodríguez, Alba
A1 González Núñez, María Elena
A1 Mello, Rosella
A1 Muñoz, Bianca K.
A1 Ojo, Wilfried-Solo
A1 Asensio, Gregorio
A1 Etienne, Michel
A1 Pérez Romero, Pedro José
AB Even in the context of hydrocarbons’ general resistance to selective functionalization, methane’svolatility and strong bonds pose a particular challenge. We report here that silver complexesbearing perfluorinated indazolylborate ligands catalyze the reaction of methane (CH4) with ethyldiazoacetate (N2CHCO2Et) to yield ethyl propionate (CH3CH2CO2Et). The use of supercritical carbondioxide (scCO2) as the solvent is key to the reaction’s success. Although the catalyst is onlysparingly soluble in CH4/CO2 mixtures, optimized conditions presently result in a 19% yield ofethyl propionate (based on starting quantity of the diazoester) at 40°C over 14 hours.
PB American Association for the Advancement of Science
SN 0036-8075
SN 1095-9203 (electrónico)
YR 2011
FD 2011-05
LK http://hdl.handle.net/10272/11557
UL http://hdl.handle.net/10272/11557
LA eng
NO Caballero Bevia, A., Despagnet-Ayoub, E., Díaz Requejo, M.M., Díaz Rodríguez, A., González Núñez, M.E., Mello, R., Muñoz, Bianca K., Ojo, W-S., Asensio, G.,  Etienne, M., Pérez Romero, P.J.: "Silver-Catalyzed C-C Bond Formation Between Methane and Ethyl Diazoacetate in Supercritical CO2". Science. Vol. 332 n. 6031 págs. 835-838, (2011). DOI: 10.1126/science.1204131
NO We dedicate this work to Professor Ernesto Carmona. Support for this work was provided by the Ministerio de Ciencia e Innovacion (grants CTQ2008-00042-BQU, CTQ2007-65251-BQU, and CTQ2007-30762-E), the European Research Area Chemistry Programme (2nd call "Chemical activation of carbon dioxide and methane" contract no. 1736154), the Consolider Ingenio 2010 (grants CSD2006-003 and CSD2007-00006), the Institut de Chimie of the CNRS, the Junta de Andalucia (P07-FQM-2870), and the Generalitat Velenciana (ACOMP/2010/155). We thank the Servicio Central de Soporte a la Investigacion Experimental (Universidad de Valencia) for access to the instrumental facilities and J. de la Rosa and A. Sanchez de la Campa (Universidad de Huelva) for ICP-MS analyses.Ministerio de Ciencia e Innovación (grantsCTQ2008-00042-BQU, CTQ2007-65251-BQU, andCTQ2007-30762-E), the European Research AreaChemistry Programme (2nd call “Chemical activation ofcarbon dioxide and methane” contract no. 1736154), theConsolider Ingenio 2010 (grants CSD2006-003 andCSD2007-00006), the Institut de Chimie of the CNRS, theJunta de Andalucía (P07-FQM-2870), and the GeneralitatVelenciana (ACOMP/2010/155).
DS Repositorio Institucional de la Universidad de Huelva
RD 30 may 2026