Abstract
Gas phase studies offer an ideal medium whereby structural and reactivity properties of charged species may be unveiled in the absence of solvent, matrix or counterion effects. In this environment NO binds to iron(II)- and iron(III)-hemes with comparable kinetics and equilibrium parameters, conclusively elucidating the factors determining the widely different affinity in protic solvents or in heme proteins. IRMPD spectroscopy of the isolated species provides unambiguous characterization of the gaseous nitrosyl heme complexes.
Highlights
In the past few decades inorganic, small molecules (NO, CO, H2S), once considered primarily as toxic gases, have been discovered to be endogenously formed and to play an important role as signaling molecules.[1]
The comparative examination of the kinetics and thermodynamic parameters for the association reaction of iron(II)- and iron(III) heme ions to NO has been thoroughly investigated in the gas phase and the major results are reported in the present feature article
The kinetic and thermodynamic data characterizing these systems in the dilute gas phase are unaffected by external factors due to the presence of solvent, counterions, protein matrix, π−π aggregates, and axial ligands
Summary
In the past few decades inorganic, small molecules (NO, CO, H2S), once considered primarily as toxic gases, have been discovered to be endogenously formed and to play an important role as signaling molecules.[1]. J. Ignarro has given worldwide recognition to the vast array of functions performed by this unique simple molecule.[3−5] Nitric oxide is responsible for several physiological activities in mammalian biology. Ignarro has given worldwide recognition to the vast array of functions performed by this unique simple molecule.[3−5] Nitric oxide is responsible for several physiological activities in mammalian biology It is an important mediator in cell signaling, blood flow regulation and immune response. The significant information that can be obtained from isolating a charged species from counter ion, solvent or matrix, has been appreciated by Professor Mirjana Eckert-Maksic and taken advantage of in her seminal studies providing new insight into several aspects of physical organic chemistry.[13−19] In grateful recognition of the valuable contribution of a distinguished scientist and esteemed friend, we are dedicating an overview of our work on the heme-NO interaction focused on both reactivity and structural and spectroscopic issues
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