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- ItemImpact of methane and black carbon mitigation on forcing and temperature: a multi-model scenario analysis(Dordrecht [u.a.] : Springer Science + Business Media B.V, 2020) Smith, Steven J.; Chateau, Jean; Dorheim, Kalyn; Drouet, Laurent; Durand-Lasserve, Olivier; Fricko, Oliver; Fujimori, Shinichiro; Hanaoka, Tatsuya; Harmsen, Mathijs; Hilaire, Jérôme; Keramidas, Kimon; Klimont, Zbigniew; Luderer, Gunnar; Moura, Maria Cecilia P.; Riahi, Keywan; Rogelj, Joeri; Sano, Fuminori; van Vuuren, Detlef P.; Wada, KenichiThe relatively short atmospheric lifetimes of methane (CH4) and black carbon (BC) have focused attention on the potential for reducing anthropogenic climate change by reducing Short-Lived Climate Forcer (SLCF) emissions. This paper examines radiative forcing and global mean temperature results from the Energy Modeling Forum (EMF)-30 multi-model suite of scenarios addressing CH4 and BC mitigation, the two major short-lived climate forcers. Central estimates of temperature reductions in 2040 from an idealized scenario focused on reductions in methane and black carbon emissions ranged from 0.18–0.26 °C across the nine participating models. Reductions in methane emissions drive 60% or more of these temperature reductions by 2040, although the methane impact also depends on auxiliary reductions that depend on the economic structure of the model. Climate model parameter uncertainty has a large impact on results, with SLCF reductions resulting in as much as 0.3–0.7 °C by 2040. We find that the substantial overlap between a SLCF-focused policy and a stringent and comprehensive climate policy that reduces greenhouse gas emissions means that additional SLCF emission reductions result in, at most, a small additional benefit of ~ 0.1 °C in the 2030–2040 time frame. © 2020, Battelle Memorial Institute.
- ItemEnhancement and limits of the selective oxidation of methane to formaldehyde over V-SBA-15: Influence of water cofeed and product decomposition(Amsterdam : Elsevier, 2021) Kunkel, Benny; Wohlrab, SebastianThe possibility of a selective catalytic oxidation of methane to formaldehyde has been known for decades, and positive influences of water added to the reaction mixture and ultra-short contact times have been reported. In the present work, the complexity of interdependencies has been revealed. Specific parameter variations can increase conversion and selectivity of the target product. Surprisingly, formaldehyde formation over VOx species and its decomposition in gas phase were equally dependent on the partial pressure of the added water, so that the sweet spot can only be found by varying the residence time. © 2021 The Author(s)
- ItemImpact of energy crop rotation design on multiple aspects of resource efficiency(Hoboken, NJ : Wiley, 2016) Peter, Christiane; Glemnitz, Michael; Winter, Katharina; Kornatz, Peter; Müller, Janine; Heiermann, Monika; Aurbacher, JoachimBiogas production can cause environmental problems due to a biased alignment of one energy crop used as a feedstock, e.g., maize in Germany. Diversification of crop rotations and resource-efficient management can be the key to sustainable crop management. Four crop rotations on eight sites across Germany were evaluated in terms of their resource efficiency (area use, energy, and economic efficiency) to derive options. Analysis revealed high variation in all indicators under review, with a high variance explanation by the interaction between crop rotation and regional characteristics. Furthermore, results indicate that high area-specific methane yields do not equate to high energy efficiency. Crop management adaptation is a useful tool for optimizing resource efficiency.
- ItemDecomposition of methane over alumina supported Fe and Ni–Fe bimetallic catalyst: Effect of preparation procedure and calcination temperature(Amsterdam [u.a.] : Elsevier, 2016) Al-Fatesh, A.S.; Fakeeha, A.H.; Ibrahim, A.A.; Khan, W.U.; Atia, H.; Eckelt, R.; Seshan, K.; Chowdhury, B.Catalytic decomposition of methane has been studied extensively as the production of hydrogen and formation of carbon nanotube is proven crucial from the scientific and technological point of view. In that context, variation of catalyst preparation procedure, calcination temperature and use of promoters could significantly alter the methane conversion, hydrogen yield and morphology of carbon nanotubes formed after the reaction. In this work, Ni promoted and unpromoted Fe/Al2O3 catalysts have been prepared by impregnation, sol–gel and co-precipitation method with calcination at two different temperatures. The catalysts were characterized by X-ray diffraction (XRD), N2 physisorption, temperature programmed reduction (TPR) and thermogravimetric analysis (TGA) techniques. The catalytic activity was tested for methane decomposition reaction. The catalytic activity was high when calcined at 500 °C temperature irrespective of the preparation method. However while calcined at high temperature the catalyst prepared by impregnation method showed a high activity. It is found from XRD and TPR characterization that disordered iron oxides supported on alumina play an important role for dissociative chemisorptions of methane generating molecular hydrogen. The transmission electron microscope technique results of the spent catalysts showed the formation of carbon nanotube which is having length of 32–34 nm. The Fe nanoparticles are present on the tip of the carbon nanotube and nanotube grows by contraction–elongation mechanism. Among three different methodologies impregnation method was more effective to generate adequate active sites in the catalyst surface. The Ni promotion enhances the reducibility of Fe/Al2O3 oxides showing a higher catalytic activity. The catalyst is stable up to six hours on stream as observed in the activity results.
- ItemRemote system for detection of low-levels of methane based on photonic crystal fibres and wavelength modulation spectroscopy(New York, NY : Hindawi, 2009) Carvalho, J.P.; Lehmann, H.; Bartelt, H.; Magalhes, F.; Amezcua-Correa, R.; Santos, J.L.; Roosbroeck, J.V.; Arajo, F.M.; Ferreira, L.A.; Knight, J.C.In this work we described an optical fibre sensing system for detecting low levels of methane. The properties of hollow-core photonic crystal fibres are explored to have a sensing head with favourable characteristics for gas sensing, particularly in what concerns intrinsic readout sensitivity and gas diffusion time in the sensing structure. The sensor interrogation was performed applying the Wavelength Modulation Spectroscopy technique, and a portable measurement unit was developed with performance suitable for remote detection of low levels of methane. This portable system has the capacity to simultaneously interrogate four remote photonic crystal fibre sensing heads. Copyright © 2009 J. P. Carvalho et al.
- ItemThe role of methane in future climate strategies: mitigation potentials and climate impacts(Dordrecht [u.a.] : Springer Science + Business Media B.V, 2019) Harmsen, Mathijs; Mathijs, Detlef P.; Bodirsky, Benjamin Leon; Chateau, Jean; Durand-Lasserve, Olivier; Drouet, Laurent; Fricko, Oliver; Fujimori, Shinichiro; Gernaat, David E.H.J.; Hanaoka, Tatsuya; Hilaire, Jérôme; Keramidas, Kimon; Luderer, Gunnar; Moura, Maria Cecilia P.; Sano, Fuminori; Smith, Steven J.; Wada, KenichiThis study examines model-specific assumptions and projections of methane (CH4) emissions in deep mitigation scenarios generated by integrated assessment models (IAMs). For this, scenarios of nine models are compared in terms of sectoral and regional CH4 emission reduction strategies, as well as resulting climate impacts. The models’ projected reduction potentials are compared to sector and technology-specific reduction potentials found in literature. Significant cost-effective and non-climate policy related reductions are projected in the reference case (10–36% compared to a “frozen emission factor” scenario in 2100). Still, compared to 2010, CH4 emissions are expected to rise steadily by 9–72% (up to 412 to 654 Mt CH4/year). Ambitious CO2 reduction measures could by themselves lead to a reduction of CH4 emissions due to a reduction of fossil fuels (22–48% compared to the reference case in 2100). However, direct CH4 mitigation is crucial and more effective in bringing down CH4 (50–74% compared to the reference case). Given the limited reduction potential, agriculture CH4 emissions are projected to constitute an increasingly larger share of total anthropogenic CH4 emissions in mitigation scenarios. Enteric fermentation in ruminants is in that respect by far the largest mitigation bottleneck later in the century with a projected 40–78% of total remaining CH4 emissions in 2100 in a strong (2 °C) climate policy case. © 2019, The Author(s).
- ItemFull-dimensional treatment of short-time vibronic dynamics in a molecular high-order-harmonic-generation process in methane(College Park, Md : APS, 2017) Patchkovskii, Serguei; Schuurman, Michael S.We present derivation and implementation of the multiconfigurational strong-field approximation with Gaussian nuclear wave packets (MC-SFA-GWP) - a version of the molecular strong-field approximation which treats all electronic and nuclear degrees of freedom, including their correlations, quantum mechanically. The technique allows realistic simulation of high-order-harmonic emission in polyatomic molecules without invoking reduced-dimensionality models for the nuclear motion or the electronic structure. We use MC-SFA-GWP to model isotope effects in high-order-harmonic-generation (HHG) spectroscopy of methane. The HHG emission in this molecule transiently involves the strongly vibronically coupled F22 electronic state of the CH4+ cation. We show that the isotopic HHG ratio in methane contains signatures of (a) field-free vibronic dynamics at the conical intersection (CI); (b) resonant features in the recombination cross sections; (c) laser-driven bound-state dynamics; as well as (d) the well-known short-time Gaussian decay of the emission. We assign the intrinsic vibronic feature (a) to a relatively long-lived (≥4 fs) vibronic wave packet of the singly excited ν4 (t2) and ν2 (e) vibrational modes, strongly coupled to the components of the F22 electronic state. We demonstrate that these physical effects differ in their dependence on the wavelength, intensity, and duration of the driving pulse, allowing them to be disentangled. We thus show that HHG spectroscopy provides a versatile tool for exploring both conical intersections and resonant features in photorecombination matrix elements in the regime not easily accessible with other techniques.
- ItemBiomethane Potential Test: Influence of Inoculum and the Digestion System(Basel : MDPI, 2020) Hülsemann, Benedikt; Zhou, Lijun; Merkle, Wolfgang; Hassa, Juli; Müller, Joachim; Oechsner, HansHigh precision of measurement of methane potential is important for the economic operation of biogas plants in the future. The biochemical methane potential (BMP) test based on the VDI 4630 protocol is the state-of-the-art method to determine the methane potential in Germany. The coefficient of variation (CV) of methane yield was >10% in several previous inter-laboratory tests. The aim of this work was to investigate the effects of inoculum and the digestion system on the measurement variability. Methane yield and methane percentage of five substrates were investigated in a Hohenheim biogas yield test (D-HBT) by using five inocula, which were used several times in inter- laboratory tests. The same substrates and inocula were also tested in other digestion systems. To control the quality of the inocula, the effect of adding trace elements (TE) and the microbial community was investigated. Adding TE had no influence for the selected, well- supplied inocula and the community composition depended on the source of the inocula. The CV of the specific methane yield was <4.8% by using different inocula in one D-HBT (D-HBT1) and <12.8% by using different digestion systems compared to D-HBT1. Incubation time between 7 and 14 days resulted in a deviation in CV of <4.8%.
- ItemImpact of process temperature and organic loading rate on cellulolytic/hydrolytic biofilm microbiomes during biomethanation of ryegrass silage revealed by genome-centered metagenomics and metatranscriptomics(London : BioMed Central, 2020) Maus, Irena; Klocke, Michael; Derenkó, Jaqueline; Stolze, Yvonne; Beckstette, Michael; Jost, Carsten; Wibberg, Daniel; Blom, Jochen; Henke, Christian; Willenbücher, Katharina; Rumming, Madis; Rademacher, Antje; Pühler, Alfred; Sczyrba, Alexander; Schlüter, AndreasBackground: Anaerobic digestion (AD) of protein-rich grass silage was performed in experimental two-stage two-phase biogas reactor systems at low vs. increased organic loading rates (OLRs) under mesophilic (37 °C) and thermophilic (55 °C) temperatures. To follow the adaptive response of the biomass-attached cellulolytic/hydrolytic biofilms at increasing ammonium/ammonia contents, genome-centered metagenomics and transcriptional profiling based on metagenome assembled genomes (MAGs) were conducted. Results: In total, 78 bacterial and archaeal MAGs representing the most abundant members of the communities, and featuring defined quality criteria were selected and characterized in detail. Determination of MAG abundances under the tested conditions by mapping of the obtained metagenome sequence reads to the MAGs revealed that MAG abundance profiles were mainly shaped by the temperature but also by the OLR. However, the OLR effect was more pronounced for the mesophilic systems as compared to the thermophilic ones. In contrast, metatranscriptome mapping to MAGs subsequently normalized to MAG abundances showed that under thermophilic conditions, MAGs respond to increased OLRs by shifting their transcriptional activities mainly without adjusting their proliferation rates. This is a clear difference compared to the behavior of the microbiome under mesophilic conditions. Here, the response to increased OLRs involved adjusting of proliferation rates and corresponding transcriptional activities. The analysis led to the identification of MAGs positively responding to increased OLRs. The most outstanding MAGs in this regard, obviously well adapted to higher OLRs and/or associated conditions, were assigned to the order Clostridiales (Acetivibrio sp.) for the mesophilic biofilm and the orders Bacteroidales (Prevotella sp. and an unknown species), Lachnospirales (Herbinix sp. and Kineothrix sp.) and Clostridiales (Clostridium sp.) for the thermophilic biofilm. Genome-based metabolic reconstruction and transcriptional profiling revealed that positively responding MAGs mainly are involved in hydrolysis of grass silage, acidogenesis and/or acetogenesis. Conclusions: An integrated-omics approach enabled the identification of new AD biofilm keystone species featuring outstanding performance under stress conditions such as increased OLRs. Genome-based knowledge on the metabolic potential and transcriptional activity of responsive microbiome members will contribute to the development of improved microbiological AD management strategies for biomethanation of renewable biomass. © 2020 The Author(s).
- ItemMitigation choices impact carbon budget size compatible with low temperature goals(Bristol : IOP Publishing, 2015) Rogelj, Joeri; Reisinger, Andy; McCollum, David L.; Knutti, Reto; Riahi, Keywan; Meinshausen, MalteGlobal-mean temperature increase is roughly proportional to cumulative emissions of carbon-dioxide (CO2). Limiting global warming to any level thus implies a finite CO2 budget. Due to geophysical uncertainties, the size of such budgets can only be expressed in probabilistic terms and is further influenced by non-CO2 emissions. We here explore how societal choices related to energy demand and specific mitigation options influence the size of carbon budgets for meeting a given temperature objective. We find that choices that exclude specific CO2 mitigation technologies (like Carbon Capture and Storage) result in greater costs, smaller compatible CO2 budgets until 2050, but larger CO2 budgets until 2100. Vice versa, choices that lead to a larger CO2 mitigation potential result in CO2 budgets until 2100 that are smaller but can be met at lower costs. In most cases, these budget variations can be explained by the amount of non-CO2 mitigation that is carried out in conjunction with CO2, and associated global carbon prices that also drive mitigation of non-CO2 gases. Budget variations are of the order of 10% around their central value. In all cases, limiting warming to below 2 °C thus still implies that CO2 emissions need to be reduced rapidly in the coming decades.