https://works.bepress.com/derek_lovley/344/download/

Hydrogen concentrations as an indicator of the predominant terminal electron-accepting reactions in aquatic sediments

There is much interest in biogeochemical processes that occur at the interface between soils and streams since, at the scale of landscapes, these habitats may function as control points for fluxes of nitrogen (N) and other nutrients from terrestrial to aquatic ecosystems. Here we examine whether a thermodynamic perspective can enhance our mechanistic and predictive understanding of the biogeochemical function of soil-stream interfaces, by considering how microbial communities interact with variations in supplies of electron donors and acceptors. Over a two-year period we analyzed >1400 individual samples of subsurface waters from networks of sample wells in riparian wetlands along Smith Creek, a first-order stream draining a mixed forested-agricultural landscape in southwestern Michigan, USA. We focused on areas where soil water and ground water emerged into the stream, and where we could characterize subsurface flow paths by measures of hydraulic head and/or by in situ additions of hydrologic tracers. We found strong support for the idea that the biogeochemical function of soil-stream interfaces is a predictable outcome of the interaction between microbial communities and supplies of electron donors and acceptors. Variations in key electron donors and acceptors (NO 3 - , N 2 O, NH 4 + , SO 4 2- , CH 4 , and dissolved organic carbon [DOC]) closely followed predictions from thermodynamic theory. Transformations of N and other elements resulted from the response of microbial communities to two dominant hydrologic flow paths: (1) horizontal flow of shallow subsurface waters with high levels of electron donors (i.e., DOC, CH 4 , and NH 4 + ), and (2) near-stream vertical upwelling of deep subsurface waters with high levels of energetically favorable electron acceptors (i.e., NO 3 - , N 2 O, and SO 4 2- ). Our results support the popular notion that soil-stream interfaces can possess strong potential for removing dissolved N by denitrification. Yet in contrast to prevailing ideas, we found that denitrification did not consume all NO 3 - that reached the soil-stream interface via subsurface flow paths. Analyses of subsurface N chemistry and natural abundances of δ 15 N in NO 3 - and NH 4 + suggested a narrow near-stream region as functionally the most important location for NO 3 - consumption by denitrification. This region was characterized by high throughput of terrestrially derived water, by accumulation of dissolved NO 3 - and N 2 O, and by low levels of DOC. Field experiments supported our hypothesis that the sustained ability for removal of dissolved NO 3 - and N 2 O should be limited by supplies of oxidizable carbon via shallow flowpaths. In situ additions of acetate, succinate, and propionate induced rates of NO 3 - removal (∼1.8 g N.m -2 .d -1 ) that were orders of magnitude greater than typically reported from riparian habitats. We propose that the immediate near-stream region may be especially important for determining the landscape-level function of many riparian wetlands. Management efforts to optimize the removal of NO 3 - by denitrification ought to consider promoting natural inputs of oxidizable carbon to this near-stream region.

/pdf/thermodynamic-constraints-on-nitrogen-transformations-and-1mlizzo449.pdf

Thermodynamic constraints on nitrogen transformations and other biogeochemical processes at soil-stream interfaces

There is much interest in biogeochemical processes that occur at the interface between soils and streams since, at the scale of landscapes, these habitats may function as control points for fluxes of nitrogen (N) and other nutrients from terrestrial to aquatic ecosystems. Here we examine whether a thermodynamic perspective can enhance our mechanistic and predictive understanding of the biogeochemical function of soil–stream interfaces, by considering how microbial communities interact with variations in supplies of electron donors and acceptors. Over a two-year period we analyzed >1400 individual samples of subsurface waters from networks of sample wells in riparian wetlands along Smith Creek, a first-order stream draining a mixed forested–agricultural landscape in southwestern Michigan, USA. We focused on areas where soil water and ground water emerged into the stream, and where we could characterize subsurface flow paths by measures of hydraulic head and/or by in situ additions of hydrologic tracers.

We found strong support for the idea that the biogeochemical function of soil–stream interfaces is a predictable outcome of the interaction between microbial communities and supplies of electron donors and acceptors. Variations in key electron donors and acceptors (NO3−, N2O, NH4+, SO42−, CH4, and dissolved organic carbon [DOC]) closely followed predictions from thermodynamic theory. Transformations of N and other elements resulted from the response of microbial communities to two dominant hydrologic flow paths: (1) horizontal flow of shallow subsurface waters with high levels of electron donors (i.e., DOC, CH4, and NH4+), and (2) near-stream vertical upwelling of deep subsurface waters with high levels of energetically favorable electron acceptors (i.e., NO3−, N2O, and SO42−).

Our results support the popular notion that soil–stream interfaces can possess strong potential for removing dissolved N by denitrification. Yet in contrast to prevailing ideas, we found that denitrification did not consume all NO3− that reached the soil–stream interface via subsurface flow paths. Analyses of subsurface N chemistry and natural abundances of δ15N in NO3− and NH4+ suggested a narrow near-stream region as functionally the most important location for NO3− consumption by denitrification. This region was characterized by high throughput of terrestrially derived water, by accumulation of dissolved NO3− and N2O, and by low levels of DOC. Field experiments supported our hypothesis that the sustained ability for removal of dissolved NO3− and N2O should be limited by supplies of oxidizable carbon via shallow flowpaths. In situ additions of acetate, succinate, and propionate induced rates of NO3− removal (∼1.8 g N·m−2·d−1) that were orders of magnitude greater than typically reported from riparian habitats. We propose that the immediate near-stream region may be especially important for determining the landscape-level function of many riparian wetlands. Management efforts to optimize the removal of NO3− by denitrification ought to consider promoting natural inputs of oxidizable carbon to this near-stream region.

Thermodynamic constraints on nitrogentransformations and other biogeochemicalprocesses at soil–stream interfaces

The advent of renewable energy conversion systems exacerbates the existing issue of intermittent excess power. Microbial electrosynthesis can use this power to capture CO2 and produce multicarbon compounds as a form of energy storage. As catalysts, microbial populations can be used, provided side reactions such as methanogenesis are avoided. Here a simple but effective approach is presented based on enrichment of a robust microbial community via several culture transfers with H2:CO2 conditions. This culture produced acetate at a concentration of 1.29 ± 0.15 g L–1 (maximum up to 1.5 g L–1; 25 mM) from CO2 at a fixed current of −5 Am–2 in fed-batch bioelectrochemical reactors at high N2:CO2 flow rates. Continuous supply of reducing equivalents enabled acetate production at a rate of 19 ± 2 gm–2d–1 (projected cathode area) in several independent experiments. This is a considerably high rate compared with other unmodified carbon-based cathodes. 58 ± 5% of the electrons was recovered in acetate, whereas 30 ± 1...

https://biblio.ugent.be/publication/6884952/file/6884955.pdf

Selective Enrichment Establishes a Stable Performing Community for Microbial Electrosynthesis of Acetate from CO2

Extraordinary 13C enrichment of diether lipids at the Lost City Hydrothermal Field indicates a carbon-limited ecosystem

The apparent Ks values for H2 of several phylogenetically distant strains of both methanogenic bacteria and sulfate-reducing bacteria were measured. The sulfate reducers had Ks values of about 2 μM whereas the Ks values of the methanogens were 6–20 μM. This indicates that probably all sulfate-reducing bacteria have a higher substrate affinity for H2 than the methanogenic bacteria. Difference in substrate affinity can thus account for the inhibition of methanogenesis from H2 and CO2 in sulfate-rich ecosystems (mainly saltwater marshes), where the H2 concentration is well below 5 μM. Possible explanations for this general phenomenon are discussed.

J. K. Kristjansson

Papers

Why do sulfate-reducing bacteria outcompete methanogenic bacteria for substrates?