Publications by Colleges and Departments (MSU - Bozeman)
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Item Does boron or nitrogen substitution affect hydrogen physisorption on open carbon surfaces?(Royal Society of Chemistry, 2022-01) Rowsey, Rylan; Taylor, Erin E.; Hinson, Ryan W.; Compton, Dalton; Stadie, Nicholas P.; SzilagyiIncorporation of heteroatoms in carbon materials is commonly expected to influence their physical or chemical properties. However, contrary to previous results for methane adsorption, no technologically significant effect was identified for the hydrogen physisorption energies (measured 4.1–4.6 kJ mol−1 and calculated qst = −ΔHads = 4.1 ± 0.7 kJ mol−1 using a comprehensive set of levels of theory) as a function of B- and N-substitution of a mid-plane C-site on open carbon surfaces.Item Investigating Abiotic and Biotic Mechanisms of Pyrite Reduction(Frontiers Media SA, 2022-05) Lange Spietz, Rachel K.; Payne, Devon; Kulkarni, Gargi; Metcalf, William W.; Roden, Eric E.; Boyd, Eric S.Pyrite (FeS2) has a very low solubility and therefore has historically been considered a sink for iron (Fe) and sulfur (S) and unavailable to biology in the absence of oxygen and oxidative weathering. Anaerobic methanogens were recently shown to reduce FeS2 and assimilate Fe and S reduction products to meet nutrient demands. However, the mechanism of FeS2 mineral reduction and the forms of Fe and S assimilated by methanogens remained unclear. Thermodynamic calculations described herein indicate that H2 at aqueous concentrations as low as 10–10 M favors the reduction of FeS2, with sulfide (HS–) and pyrrhotite (Fe1–xS) as products; abiotic laboratory experiments confirmed the reduction of FeS2 with dissolved H2 concentrations greater than 1.98 × 10–4 M H2. Growth studies of Methanosarcina barkeri provided with FeS2 as the sole source of Fe and S resulted in H2 production but at concentrations too low to drive abiotic FeS2 reduction, based on abiotic laboratory experimental data. A strain of M. barkeri with deletions in all [NiFe]-hydrogenases maintained the ability to reduce FeS2 during growth, providing further evidence that extracellular electron transport (EET) to FeS2 does not involve H2 or [NiFe]-hydrogenases. Physical contact between cells and FeS2 was required for mineral reduction but was not required to obtain Fe and S from dissolution products. The addition of a synthetic electron shuttle, anthraquinone-2,6-disulfonate, allowed for biological reduction of FeS2 when physical contact between cells and FeS2 was prohibited, indicating that exogenous electron shuttles can mediate FeS2 reduction. Transcriptomics experiments revealed upregulation of several cytoplasmic oxidoreductases during growth of M. barkeri on FeS2, which may indicate involvement in provisioning low potential electrons for EET to FeS2. Collectively, the data presented herein indicate that reduction of insoluble FeS2 by M. barkeri occurred via electron transfer from the cell surface to the mineral surface resulting in the generation of soluble HS– and mineral-associated Fe1–xS. Solubilized Fe(II), but not HS–, from mineral-associated Fe1–xS reacts with aqueous HS– yielding aqueous iron sulfur clusters (FeSaq) that likely serve as the Fe and S source for methanogen growth and activity. FeSaq nucleation and subsequent precipitation on the surface of cells may result in accelerated EET to FeS2, resulting in positive feedback between cell activity and FeS2 reduction.Item Toward Better Genetically Encoded Sensors of Membrane Potential(2016-03) Urschel, Matthew R.; Hamilton, Trinity L.; Roden, Eric E.; Boyd, Eric S.Facultative autotrophs are abundant components of communities inhabiting geothermal springs. However, the influence of uptake kinetics and energetics on preference for substrates is not well understood in this group of organisms. Here, we report the isolation of a facultatively autotrophic crenarchaeote, strain CP80, from Cinder Pool (CP, 88.7°C, pH 4.0), Yellowstone National Park. The 16S rRNA gene sequence from CP80 is 98.8% identical to that from Thermoproteus uzonensis and is identical to the most abundant sequence identified in CP sediments. Strain CP80 reduces elemental sulfur (S8°) and demonstrates hydrogen (H2)-dependent autotrophic growth. H2-dependent autotrophic activity is suppressed by amendment with formate at a concentration in the range of 20–40 μM, similar to the affinity constant determined for formate utilization. Synthesis of a cell during growth with low concentrations of formate required 0.5 μJ compared to 2.5 μJ during autotrophic growth with H2. These results, coupled to data indicating greater C assimilation efficiency when grown with formate as compared to carbon dioxide, are consistent with preferential use of formate for energetic reasons. Collectively, these results provide new insights into the kinetic and energetic factors that influence the physiology and ecology of facultative autotrophs in high-temperature acidic environments.