Although the mineral dolomite is abundant in ancient lowtemperature sedimentary systems, it is scarce in modern systems below 50°C. Chemical mechanism(s) enhancing its formation remain an enigma because abiotic dolomite has been challenging to synthesize at low temperature in laboratory settings. Microbial enhancement of dolomite precipitation at low temperature has been reported; however, it is still unclear exactly how microorganisms influence reaction kinetics. Here we document the abiotic synthesis of low-temperature dolomite in laboratory experiments and constrain possible mechanisms for dolomite formation. Ancient and modern seawater solution compositions, with identical pH and pCO 2 , were used to precipitate an ordered, stoichiometric dolomite phase at 30°C in as few as 20 d. Mg-rich phases nucleate exclusively on carboxylated polystyrene spheres along with calcite, whereas aragonite forms in solution via homogeneous nucleation. We infer that Mg ions are complexed and dewatered by surface-bound carboxyl groups, thus decreasing the energy required for carbonation. These results indicate that natural surfaces, including organic matter and microbial biomass, possessing a high density of carboxyl groups may be a mechanism by which ordered dolomite nuclei form. Although environments rich in organic matter may be of interest, our data suggest that sharp biogeochemical interfaces that promote microbial death, as well as those with high salinity may, in part, control carboxyl-group density on organic carbon surfaces, consistent with origin of dolomites from microbial biofilms, as well as hypersaline and mixing zone environments.biomineralization | carbonates A lthough synthesis of dolomite in laboratory settings at high temperature (80-250°C) has yielded valuable information regarding dolomite formation (1, 2), the validity of extrapolating kinetic data at 250°C down to 25°C is questionable. Synthesis of low-temperature dolomite is hindered by slow reaction kinetics (2). Kinetic inhibition is attributed to lack of solution supersaturation (3), sulfate inhibition (1), cation desolvation (4), and lack of nucleation sites (5). Laboratory precipitation at low temperature has only been successful in producing disordered dolomite: from solutions with high salinity (6); through intermittent (7) or complete dehydration (8); by using organic or inorganic compounds that effectively dewater Mg 2+ ions (9-11); or in the presence of microorganisms, their exudates, or surfaces (12, 13).Microbial dolomite has been produced in the presence of several different metabolic pathways including sulfate reduction, methanogenesis, methanotrophy, sulfide oxidation, and aerobic respiration (12-16), which may drive precipitation through the supersaturation of solutions with respect to dolomite. Recent work, however, has focused on the role of microbial cells and exopolymeric substances (EPS) as surfaces for dolomite nucleation (17). Whereas these studies clearly demonstrate that these surfaces are involved in dolomite formation, specific ...
Here we report precipitation of dolomite at low temperature (30 degrees C) mediated by a mixed anaerobic microbial consortium composed of dissimilatory iron-reducing bacteria (DIRB), fermenters, and methanogens. Initial solution geochemistry is controlled by DIRB, but after 90 days shifts to a system dominated by methanogens. In live experiments conditions are initially saturated with respect to dolomite (Omega(dol) = 19.40) and increase by two orders of magnitude (Omega(dol) = 2 330.77) only after the onset of methanogenesis, as judged by the increasing [CH(4)] and the detection of methanogenic micro-organisms. We identify ordered dolomite in live microcosms after 90 days via powder X-ray diffraction, while sterile controls precipitate only calcite. Scanning electron microscopy and transmitted electron microscopy demonstrate that the precipitated dolomite is closely associated with cell walls and putative extra-cellular polysaccharides. Headspace gas measurements and denaturing gradient gel electrophoresis confirm the presence of both autotrophic and acetoclastic methanogens and exclude the presence of DIRB and sulfate-reducing bacteria after dolomite begins forming. Furthermore, the absence of dolomite in the controls and prior to methanogenesis confirm that methanogenic Archaea are necessary for the low-temperature precipitation of dolomite under the experimental conditions tested.
This study formulates a comprehensive depositional model for hydromagnesite-magnesite playas. Mineralogical, isotopic and hydrogeochemical data are coupled with electron microscopy and field observations of the hydromagnesite-magnesite playas near Atlin, British Columbia, Canada. Four surface environments are recognized: wetlands, grasslands, localized mounds (metrescale) and amalgamated mounds composed primarily of hydromagnesite [Mg 5 (CO 3 ) 4 (OH) 2 Á4H 2 O], which are interpreted to represent stages in playa genesis. Water chemistry, precipitation kinetics and depositional environment are primary controls on sediment mineralogy. At depth (average % 2 m), CaMg-carbonate sediments overlay early Holocene glaciolacustrine sediments indicating deposition within a lake post-deglaciation. This mineralogical change corresponds to a shift from siliciclastic to chemical carbonate deposition as the supply of fresh surface water (for example, glacier meltwater) ceased and was replaced by alkaline groundwater. Weathering of ultramafic bedrock in the region produces Mg-HCO 3 groundwater that concentrates by evaporation upon discharging into closed basins, occupied by the playas. An uppermost unit of Mg-carbonate sediments (hydromagnesite mounds) overlies the Ca-Mg-carbonate sediments. This second mineralogical shift corresponds to a change in the depositional environment from subaqueous to subaerial, occurring once sediments 'emerged' from the water surface. Capillary action and evaporation draw Mg-HCO 3 water up towards the ground surface, precipitating Mg-carbonate minerals. Evaporation at the water table causes precipitation of lansfordite [MgCO 3 Á5H 2 O] which partially cements pre-existing sediments forming a hardpan. As carbonate deposition continues, the weight of the overlying sediments causes compaction and minor lateral movement of the mounds leading to amalgamation of localized mounds. Radiocarbon dating of buried vegetation at the Ca-Mg-carbonate boundary indicates that there has been ca 8000 years of continuous Mg-carbonate deposition at a rate of 0Á4 mm yr À1 . The depositional model accounts for the many sedimentological, mineralogical and geochemical processes that occur in the four surface environments; elucidating past and present carbonate deposition.
Photoferrotrophs repel iron to deposit banded iron formations and contribute methane to the atmosphere during the Archean Eon.
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