Počet záznamů: 1  

Mono- and binuclear non-heme iron chemistry from a theoretical perspective

  1. 1. 0463791 - UOCHB-X 2017 RIV DE eng J - Článek v odborném periodiku
    Rokob, T. A. - Chalupský, Jakub - Bím, Daniel - Andrikopoulos, Prokopis C. - Srnec, Martin - Rulíšek, Lubomír
    Mono- and binuclear non-heme iron chemistry from a theoretical perspective.
    Journal of Biological Inorganic Chemistry. Roč. 21, 5/6 (2016), s. 619-644. ISSN 0949-8257
    Grant CEP: GA ČR(CZ) GJ15-10279Y; GA ČR(CZ) GA14-31419S; GA ČR GA15-19143S
    Grant ostatní:COST(XE) CM1305
    Institucionální podpora: RVO:61388963 ; RVO:61388955
    Klíčová slova: non-heme iron * density functional theory * multireference methods * dioxygen activation * reactivity
    Kód oboru RIV: CF - Fyzikální chemie a teoretická chemie
    Impakt faktor: 2.894, rok: 2016

    In this minireview, we provide an account of the current state-of-the-art developments in the area of mono- and binuclear non-heme enzymes (NHFe and NHFe2) and the smaller NHFe(2) synthetic models, mostly from a theoretical and computational perspective. The sheer complexity, and at the same time the beauty, of the NHFe(2) world represents a challenge for experimental as well as theoretical methods. We emphasize that the concerted progress on both theoretical and experimental side is a conditio sine qua non for future understanding, exploration and utilization of the NHFe(2) systems. After briefly discussing the current challenges and advances in the computational methodology, we review the recent spectroscopic and computational studies of NHFe(2) enzymatic and inorganic systems and highlight the correlations between various experimental data (spectroscopic, kinetic, thermodynamic, electrochemical) and computations. Throughout, we attempt to keep in mind the most fascinating and attractive phenomenon in the NHFe(2) chemistry, which is the fact that despite the strong oxidative power of many reactive intermediates, the NHFe(2) enzymes perform catalysis with high selectivity. We conclude with our personal viewpoint and hope that further developments in quantum chemistry and especially in the field of multireference wave function methods are needed to have a solid theoretical basis for the NHFe(2) studies, mostly by providing benchmarking and calibration of the computationally efficient and easy-to-use DFT methods.
    Trvalý link: http://hdl.handle.net/11104/0262886