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- ItemDirect raman spectroscopic measurements of biological nitrogen fixation under natural conditions: An analytical approach for studying nitrogenase activity(Columbus, Ohio : American Chemical Society, 2016) Jochum, Tobias; Fastnacht, Agnes; Trumbore, Susan E.; Popp, Jürgen; Frosch, TorstenBiological N2 fixation is a major input of bioavailable nitrogen, which represents the most frequent factor limiting the agricultural production throughout the world. Especially, the symbiotic association between legumes and Rhizobium bacteria can provide substantial amounts of nitrogen (N) and reduce the need for industrial fertilizers. Despite its importance in the global N cycle, rates of biological nitrogen fixation have proven difficult to quantify. In this work, we propose and demonstrate a simple analytical approach to measure biological N2 fixation rates directly without a proxy or isotopic labeling. We determined a mean N2 fixation rate of 78 ± 5 μmol N2 (g dry weight nodule)-1 h-1 of a Medicago sativa-Rhizobium consortium by continuously analyzing the amount of atmospheric N2 in static environmental chambers with Raman gas spectroscopy. By simultaneously analyzing the CO2 uptake and photosynthetic plant activity, we think that a minimum CO2 mixing ratio might be needed for natural N2 fixation and only used the time interval above this minimum CO2 mixing ratio for N2 fixation rate calculations. The proposed approach relies only on noninvasive measurements of the gas phase and, given its simplicity, indicates the potential to estimate biological nitrogen fixation of legume symbioses not only in laboratory experiments. The same methods can presumably also be used to detect N2 fluxes by denitrification from ecosystems to the atmosphere. (Figure Presented).
- ItemRevolutions in energy input and material cycling in Earth history and human history(München : European Geopyhsical Union, 2016) Lenton, Timothy M.; Pichler, Peter-Paul; Weisz, HelgaMajor revolutions in energy capture have occurred in both Earth and human history, with each transition resulting in higher energy input, altered material cycles and major consequences for the internal organization of the respective systems. In Earth history, we identify the origin of anoxygenic photosynthesis, the origin of oxygenic photosynthesis, and land colonization by eukaryotic photosynthesizers as step changes in free energy input to the biosphere. In human history we focus on the Palaeolithic use of fire, the Neolithic revolution to farming, and the Industrial revolution as step changes in free energy input to human societies. In each case we try to quantify the resulting increase in energy input, and discuss the consequences for material cycling and for biological and social organization. For most of human history, energy use by humans was but a tiny fraction of the overall energy input to the biosphere, as would be expected for any heterotrophic species. However, the industrial revolution gave humans the capacity to push energy inputs towards planetary scales and by the end of the 20th century human energy use had reached a magnitude comparable to the biosphere. By distinguishing world regions and income brackets we show the unequal distribution in energy and material use among contemporary humans. Looking ahead, a prospective sustainability revolution will require scaling up new renewable and decarbonized energy technologies and the development of much more efficient material recycling systems – thus creating a more autotrophic social metabolism. Such a transition must also anticipate a level of social organization that can implement the changes in energy input and material cycling without losing the large achievements in standard of living and individual liberation associated with industrial societies.
- ItemTwo-photon, visible light water splitting at a molecular ruthenium complex(Cambridge : RSC Publ., 2021) Schneidewind, Jacob; Argüello Cordero, Miguel A.; Junge, Henrik; Lochbrunner, Stefan; Beller, MatthiasWater splitting to give molecular oxygen and hydrogen or the corresponding protons and electrons is a fundamental four-electron redox process, which forms the basis of photosynthesis and is a promising approach to convert solar into chemical energy. Artificial water splitting systems have struggled with orchestrating the kinetically complex absorption of four photons as well as the difficult utilization of visible light. Based on a detailed kinetic, spectroscopic and computational study of Milstein's ruthenium complex, we report a new mechanistic paradigm for water splitting, which requires only two photons and offers a new method to extend the range of usable wavelengths far into the visible region. We show that two-photon water splitting is enabled by absorption of the first, shorter wavelength photon, which produces an intermediate capable of absorbing the second, longer wavelength photon (up to 630 nm). The second absorption then causes O–O bond formation and liberation of O2. Theoretical modelling shows that two-photon water splitting can be used to achieve a maximum solar-to-hydrogen efficiency of 18.8%, which could be increased further to 28.6% through photochemical instead of thermal H2 release. It is therefore possible to exceed the maximum efficiency of dual absorber systems while only requiring a single catalyst. Due to the lower kinetic complexity, intrinsic utilization of a wide wavelength range and high-performance potential, we believe that this mechanism will inspire the development of a new class of water splitting systems that go beyond the reaction blueprint of photosynthesis.
- ItemComprehensive Assessment of the Dynamics of Banana Chilling Injury by Advanced Optical Techniques(Basel : MDPI, 2021) Herppich, Werner B.; Zsom, TamásGreen‐ripe banana fruit are sensitive to chilling injury (CI) and, thus, prone to postharvest quality losses. Early detection of CI facilitates quality maintenance and extends shelf life. CI affects all metabolic levels, with membranes and, consequently, photosynthesis being primary targets. Optical techniques such as chlorophyll a fluorescence analysis (CFA) and spectroscopy are promising tools to evaluate CI effects in photosynthetically active produce. Results obtained on bananas are, however, largely equivocal. This results from the lack of a rigorous evaluation of chilling impacts on the various aspects of photosynthesis. Continuous and modulated CFA and imaging (CFI), and VIS remission spectroscopy (VRS) were concomitantly applied to noninvasively and comprehensively monitor photosynthetically relevant effects of low temperatures (5 °C, 10 °C, 11.5 °C and 13 °C). Detailed analyses of chilling‐related variations in photosynthetic activity and photoprotection, and in contents of relevant pigments in green‐ripe bananas, helped to better understand the physiological changes occurring during CI, highlighting that distinct CFA and VRS parameters comprehensively reflect various effects of chilling on fruit photosynthesis. They revealed why not all CFA parameters can be applied meaningfully for early detection of chilling effects. This study provides relevant requisites for improving CI monitoring and prediction.
- ItemAtmospheric CO2 availability induces varying responses in net photosynthesis, toxin production and N2 fixation rates in heterocystous filamentous Cyanobacteria (Nostoc and Nodularia)(Basel ; Heidelberg : Springer, 2021) Wannicke, Nicola; Herrmann, Achim; Gehringer, Michelle M.Heterocystous Cyanobacteria of the genus Nodularia form major blooms in brackish waters, while terrestrial Nostoc species occur worldwide, often associated in biological soil crusts. Both genera, by virtue of their ability to fix N2 and conduct oxygenic photosynthesis, contribute significantly to global primary productivity. Select Nostoc and Nodularia species produce the hepatotoxin nodularin and whether its production will change under climate change conditions needs to be assessed. In light of this, the effects of elevated atmospheric CO2 availability on growth, carbon and N2 fixation as well as nodularin production were investigated in toxin and non-toxin producing species of both genera. Results highlighted the following:Biomass and volume specific biological nitrogen fixation (BNF) rates were respectively almost six and 17 fold higher in the aquatic Nodularia species compared to the terrestrial Nostoc species tested, under elevated CO2 conditions.There was a direct correlation between elevated CO2 and decreased dry weight specific cellular nodularin content in a diazotrophically grown terrestrial Nostoc species, and the aquatic Nodularia species, regardless of nitrogen availability.Elevated atmospheric CO2 levels were correlated to a reduction in biomass specific BNF rates in non-toxic Nodularia species.Nodularin producers exhibited stronger stimulation of net photosynthesis rates (NP) and growth (more positive Cohen’s d) and less stimulation of dark respiration and BNF per volume compared to non-nodularin producers under elevated CO2 levels. This study is the first to provide information on NP and nodularin production under elevated atmospheric CO2 levels for Nodularia and Nostoc species under nitrogen replete and diazotrophic conditions.
- ItemConsensus model of a cyanobacterial light-dependent protochlorophyllide oxidoreductase in its pigment-free apo-form and photoactive ternary complex(London : Springer Nature, 2019) Schneidewind, Judith; Krause, Frank; Bocola, Marco; Stadler, Andreas Maximilian; Davari, Mehdi D.; Schwaneberg, Ulrich; Jaeger, Karl-Erich; Krauss, UlrichPhotosynthetic organisms employ two different enzymes for the reduction of the C17 = C18 double bond of protochlorophyllide (Pchlide), yielding the chlorophyll precursor chlorophyllide. First, a nitrogenase-like, light-independent (dark-operative) Pchlide oxidoreductase and secondly, a light-dependent Pchlide oxidoreductase (LPOR). For the latter enzyme, despite decades of research, no structural information is available. Here, we use protein structure modelling, molecular dynamics (MD) simulations combined with multi-wavelength analytical ultracentrifugation (MWA-AUC) and small angle X-ray scattering (SAXS) experiments to derive a consensus model of the LPOR apoprotein and the substrate/cofactor/LPOR ternary complex. MWA-AUC and SAXS experiments independently demonstrate that the apoprotein is monomeric, while ternary complex formation induces dimerization. SAXS-guided modelling studies provide a full-length model of the apoprotein and suggest a tentative mode of dimerization for the LPOR ternary complex, supported by published cross-link constraints. Our study provides a first impression of the LPOR structural organization.