Direkte Umwandlung von Methan zu protoniertem Formaldehyd bei Raumtemperatur in der Gasphase: Zur Rolle von Quecksilber unter den Oxidkationen der Zinktriade

Mass spectrometric analysis of the anionic products of interaction between platinum atomic anions, Pt−, and methane, CH4 and CD4, in a collision cell shows the preferred generation of [PtCH4]− and [PtCD4]− complexes and a low tendency toward dehydrogenation. [PtCH4]− is shown to be H−Pt−CH3− by a synergy between anion photoelectron spectroscopy and quantum chemical calculations, implying the rupture of a single C−H bond. The calculated reaction pathway accounts for the observed selective activation of methane by Pt−. This study presents the first example of methane activation by a single atomic anion.

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Photodissociation Mechanisms of Major Mercury(II) Species in the Atmospheric Chemical Cycle of Mercury

Francés‐Monerris

Carmona‐García

Acuña

et al. 2020

Angewandte Chemie

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Mercury is a contaminant of global concern that is transported throughout the atmosphere as elemental mercury Hg0 and its oxidized forms HgI and HgII. The efficient gas‐phase photolysis of HgII and HgI has recently been reported. However, whether the photolysis of HgII leads to other stable HgII species, to HgI, or to Hg0 and its competition with thermal reactivity remain unknown. Herein, we show that all oxidized forms of mercury rapidly revert directly and indirectly to Hg0 by photolysis. Results are based on non‐adiabatic dynamics simulations, in which the photoproduct ratios were determined with maximum errors of 3%. We construct for the first time a complete quantitative mechanism of the photochemical and thermal conversion between atmospheric HgII, HgI, and Hg0 compounds. These results reveal new fundamental chemistry that has broad implications for the global atmospheric Hg cycle. Thus, photoreduction clearly competes with thermal oxidation, with Hg0 being the main photoproduct of HgII photolysis in the atmosphere, which significantly increases the lifetime of this metal in the environment.

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Direkte Umwandlung von Methan zu protoniertem Formaldehyd bei Raumtemperatur in der Gasphase: Zur Rolle von Quecksilber unter den Oxidkationen der Zinktriade

Cited by 7 publications

References 76 publications

Neue Mitglieder und auswärtige Mitglieder der National Academy of Sciences

Neue Mitglieder und auswärtige Mitglieder der National Academy of Sciences

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

Photodissociation Mechanisms of Major Mercury(II) Species in the Atmospheric Chemical Cycle of Mercury

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