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971.
On the role of Mn(IV) vacancies in the photoreductive dissolution of hexagonal birnessite 总被引:4,自引:0,他引:4
Photoreductive dissolution of layer type Mn(IV) oxides (birnessite) under sunlight illumination to form soluble Mn(II) has been observed in both field and laboratory settings, leading to a consensus that this process is a key driver of the biogeochemical cycling of Mn in the euphotic zones of marine and freshwater ecosystems. However, the underlying mechanisms for the process remain unknown, although they have been linked to the semiconducting characteristics of hexagonal birnessite, the ubiquitous Mn(IV) oxide produced mainly by bacterial oxidation of soluble Mn(II). One of the universal properties of this biogenic mineral is the presence of Mn(IV) vacancies, long-identified as strong adsorption sites for metal cations. In this paper, the possible role of Mn vacancies in photoreductive dissolution is investigated theoretically using quantum mechanical calculations based on spin-polarized density functional theory (DFT). Our DFT study demonstrates unequivocally that Mn vacancies significantly reduce the band-gap energy for hexagonal birnessite relative to a hypothetical vacancy-free MnO2 and thus would increase the concentration of photo-induced electrons available for Mn(IV) reduction upon illumination of the mineral by sunlight. Calculations of the charge distribution in the presence of vacancies, although not fully conclusive, show a clear separation of photo-induced electrons and holes, implying a slow recombination of these charge-carriers that facilitates the two-electron reduction of Mn(IV) to Mn(II). 相似文献
972.
Jenni E. Sherriff Keith N. Wilkinson Poppy Harding Hayley Hawkins Rhys G. O. Timms Daniel S. Adler Emily J. Beverly Simon P. E. Blockley Boris Gasparyan Christina J. Manning Darren Mark Samvel Nahapetyan Katie J. Preece 《第四纪科学杂志》2022,37(1):6-27
The significance of the southern Caucasus in understanding Pleistocene hominin expansions is well established. However, the palaeoenvironments in which Palaeolithic occupation of the region took place are presently poorly defined. The Hrazdan river valley, Armenian Highlands, contains a rich Palaeolithic record alongside Middle Pleistocene volcanic, fluvial and lacustrine strata, and thus offer exciting potential for palaeoenvironmental reconstruction. We present the first results of sedimentological, geochemical, tephrostratigraphical and biological (diatoms) study of the sequence of Bird Farm 1, located in the central part of the valley. These data show six phases of landscape development during the interval 440–200 ka. The sequence represents the first quantitative Pleistocene diatom record from the Armenian Highlands and the southern Caucasus, and indicates the persistence of a deep, stratified lacustrine system, with evidence for changing lake productivity that is tentatively linked to climate. Furthermore, major element chemical characterization of visible and crypto-tephra horizons in the sequence enables the first stages of the development of a regional tephrostratigraphy. Together, the evidence from Bird Farm 1 demonstrates the importance of lacustrine archives in the region for palaeoenvironmental reconstruction and highlights the potential for linkages between archives on both a local and regional scale. 相似文献