@article{10272/11557,
year = {2011},
month = {5},
url = {http://hdl.handle.net/10272/11557},
abstract = {Even in the context of hydrocarbons’ general resistance to selective functionalization, methane’s
volatility and strong bonds pose a particular challenge. We report here that silver complexes
bearing perfluorinated indazolylborate ligands catalyze the reaction of methane (CH4) with ethyl
diazoacetate (N2CHCO2Et) to yield ethyl propionate (CH3CH2CO2Et). The use of supercritical carbon
dioxide (scCO2) as the solvent is key to the reaction’s success. Although the catalyst is only
sparingly soluble in CH4/CO2 mixtures, optimized conditions presently result in a 19% yield of
ethyl propionate (based on starting quantity of the diazoester) at 40°C over 14 hours.},
organization = {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 (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 Andalucía (P07-FQM-2870), and the Generalitat
Velenciana (ACOMP/2010/155).},
publisher = {American Association for the Advancement of Science},
keywords = {Methane activation},
keywords = {Homogeneous catalysis},
keywords = {Silver catalyst},
keywords = {Diazocompound},
keywords = {C-H functionalization},
title = {Silver-Catalyzed C-C Bond Formation between Methane and Ethyl Diazoacetate in Supercritical CO2},
doi = {10.1126/science.1204131},
author = {Caballero Bevia, Ana and Despagnet-Ayoub, Emmanuelle and Díaz Requejo, María Mar and Díaz Rodríguez, Alba and González Núñez, María Elena and Mello, Rosella and Muñoz, Bianca K. and Ojo, Wilfried-Solo and Asensio, Gregorio and Etienne, Michel and Pérez Romero, Pedro José},
}