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Thermal Hydrogen‐Atom Transfer from Methane: The Role of Radicals and Spin States in Oxo‐Cluster Chemistry
Author(s) -
Dietl Nicolas,
Schlangen Maria,
Schwarz Helmut
Publication year - 2012
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201108363
Subject(s) - radical , hydrogen atom , methane , cluster (spacecraft) , chemistry , cluster chemistry , hydrogen , thermal , atom (system on chip) , photochemistry , spin (aerodynamics) , chemical physics , physics , organic chemistry , thermodynamics , molecule , engineering , group (periodic table) , computer science , embedded system , programming language
Hydrogen‐atom transfer (HAT), as one of the fundamental reactions in chemistry, is investigated with state‐of‐the‐art gas‐phase experiments in conjunction with computational studies. The focus of this Minireview concerns the role that the intrinsic properties of gaseous oxo‐clusters play to permit HAT reactivity from saturated hydrocarbons at ambient conditions. In addition, mechanistic implications are discussed which pertain to heterogeneous catalysis. From these combined experimental/computational studies, the crucial role of unpaired spin density at the abstracting atom becomes clear, in distinct contrast to recent conclusions derived from solution‐phase experiments.