RT Journal Article
T1 An automated method to find reaction mechanisms and solve the kinetics in organometallic catalysis
A1 Varela Carrete, Jesús Ángel
A1 Vázquez Rodríguez, Saulo Ángel
A1 Martínez Núñez, Emilio
AB A novel computational method is proposed in this work for use in discovering reaction mechanisms and solving the kinetics of transition metal-catalyzed reactions. The method does not rely on either chemical intuition or assumed a priori mechanisms, and it works in a fully automated fashion. Its core is a procedure, recently developed by one of the authors, that combines accelerated direct dynamics with an efficient geometry-based post-processing algorithm to find transition states (Martinez-Nunez, E., J. Comput. Chem. 2015, 36, 222–234). In the present work, several auxiliary tools have been added to deal with the specific features of transition metal catalytic reactions. As a test case, we chose the cobalt-catalyzed hydroformylation of ethylene because of its well-established mechanism, and the fact that it has already been used in previous automated computational studies. Besides the generally accepted mechanism of Heck and Breslow, several side reactions, such as hydrogenation of the alkene, emerged from our calculations. Additionally, the calculated rate law for the hydroformylation reaction agrees reasonably well with those obtained in previous experimental and theoretical studies
PB Royal Society of Chemistry
SN 2041-6539
YR 2017
FD 2017
LK http://hdl.handle.net/10347/17542
UL http://hdl.handle.net/10347/17542
LA eng
NO Varela, J., Vázquez, S., & Martínez-Núñez, E. (2017). An automated method to find reaction mechanisms and solve the kinetics in organometallic catalysis. Chemical Science, 8(5), 3843-3851. doi: 10.1039/c7sc00549k
NO This work was supported by the Spanish MINECO (projects CTQ2014-59015R, CTQ2014-58617R and ORFEO-CINQA network CTQ2014-51912REDC), the Consellería de Cultura, the Educación e Ordenación Universitaria (project GRC2014/032 and Centro singular de investigación de Galicia accreditation 2016– 2019, ED431G/09) and the ERDF
DS Minerva
RD 25 abr 2026