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- ItemGreenhouse gas effects on the solar cycle response of water vapour and noctilucent clouds(Katlenburg, Lindau : Copernicus, 2023) Vellalassery, Ashique; Baumgarten, Gerd; Grygalashvyly, Mykhaylo; Lübken, Franz-JosefThe responses of water vapour (H2O) and noctilucent clouds (NLCs) to the solar cycle are studied using the Leibniz Institute for Middle Atmosphere (LIMA) model and the Mesospheric Ice Microphysics And tranSport (MIMAS) model. NLCs are sensitive to the solar cycle because their formation depends on background temperature and the H2O concentration. The solar cycle affects the H2O concentration in the upper mesosphere mainly in two ways: directly through the photolysis and, at the time and place of NLC formation, indirectly through temperature changes. We found that H2O concentration correlates positively with the temperature changes due to the solar cycle at altitudes above about 82 km, where NLCs form. The photolysis effect leads to an anti-correlation of H2O concentration and solar Lyman-α radiation, which gets even more pronounced at altitudes below ∼83 km when NLCs are present. We studied the H2O response to Lyman-α variability for the period 1992 to 2018, including the two most recent solar cycles. The amplitude of Lyman-α variation decreased by about 40 % in the period 2005 to 2018 compared to the preceding solar cycle, resulting in a lower H2O response in the late period. We investigated the effect of increasing greenhouse gases (GHGs) on the H2O response throughout the solar cycle by performing model runs with and without increases in carbon dioxide (CO2) and methane (CH4). The increase of methane and carbon dioxide amplifies the response of water vapour to the solar variability. Applying the geometry of satellite observations, we find a missing response when averaging over altitudes of 80 to 85 km, where H2O has a positive response and a negative response (depending on altitude), which largely cancel each other out. One main finding is that, during NLCs, the solar cycle response of H2O strongly depends on altitude.
- ItemElectrocatalytic Reduction of CO2 to Acetic Acid by a Molecular Manganese Corrole Complex(Weinheim : Wiley-VCH, 2020) De, Ratnadip; Gonglach, Sabrina; Paul, Shounik; Haas, Michael; Sreejith, S.S.; Gerschel, Philipp; Apfel, Ulf-Peter; Vuong, Thanh Huyen; Rabeah, Jabor; Roy, Soumyajit; Schöfberger, WolfgangThe controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular MnIII-corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO2. Electrochemical reduction of MnIII leads to an electroactive MnII species, which binds CO2 and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO2 to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h−1, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the MnIII-corrole center. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemFootprint-weighted tile approach for a spruce forest and a nearby patchy clearing using the ACASA model(Katlenburg-Lindau [u.a.] : Copernicus, 2018) Gatzsche, Kathrin; Babel, Wolfgang; Falge, Eva; Pyles, Rex David; Paw U., Kyaw Tha; Raabe, Armin; Foken, ThomasThe ACASA (Advanced Canopy-Atmosphere-Soil Algorithm) model, with a higher-order closure for tall vegetation, has already been successfully tested and validated for homogeneous spruce forests. The aim of this paper is to test the model using a footprint-weighted tile approach for a clearing with a heterogeneous structure of the underlying surface. The comparison with flux data shows a good agreement with a footprint-aggregated tile approach of the model. However, the results of a comparison with a tile approach on the basis of the mean land use classification of the clearing is not significantly different. It is assumed that the footprint model is not accurate enough to separate small-scale heterogeneities. All measured fluxes are corrected by forcing the energy balance closure of the test data either by maintaining the measured Bowen ratio or by the attribution of the residual depending on the fractions of sensible and latent heat flux to the buoyancy flux. The comparison with the model, in which the energy balance is closed, shows that the buoyancy correction for Bowen ratios > 1.5 better fits the measured data. For lower Bowen ratios, the correction probably lies between the two methods, but the amount of available data was too small to make a conclusion. With an assumption of similarity between water and carbon dioxide fluxes, no correction of the net ecosystem exchange is necessary for Bowen ratios > 1.5.
- ItemHow the extreme 2019-2020 Australian wildfires affected global circulation and adjustments(Katlenburg-Lindau : EGU, 2023) Senf, Fabian; Heinold, Bernd; Kubin, Anne; Müller, Jason; Schrödner, Roland; Tegen, InaWildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019-2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17ĝ€¯km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol-climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5ĝ€¯Wm-2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5ĝ€¯Wm-2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2ĝ€¯%. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.
- ItemSpatial, temporal and source contribution assessments of black carbon over the northern interior of South Africa(Katlenburg-Lindau : EGU, 2017) Chiloane, Kgaugelo Euphinia; Beukes, Johan Paul; van Zyl, Pieter Gideon; Maritz, Petra; Vakkari, Ville; Josipovic, Miroslav; Venter, Andrew Derick; Jaars, Kerneels; Tiitta, Petri; Kulmala, Markku; Wiedensohler, Alfred; Liousse, Catherine; Mkhatshwa, Gabisile Vuyisile; Ramandh, Avishkar; Laakso, LauriAfter carbon dioxide (CO2), aerosol black carbon (BC) is considered to be the second most important contributor to global warming. This paper presents equivalent black carbon (eBC) (derived from an optical absorption method) data collected from three sites in the interior of South Africa where continuous measurements were conducted, i.e. Elandsfontein, Welgegund and Marikana, as well elemental carbon (EC) (determined by evolved carbon method) data at five sites where samples were collected once a month on a filter and analysed offline, i.e. Louis Trichardt, Skukuza, Vaal Triangle, Amersfoort and Botsalano. Analyses of eBC and EC spatial mass concentration patterns across the eight sites indicate that the mass concentrations in the South African interior are in general higher than what has been reported for the developed world and that different sources are likely to influence different sites. The mean eBC or EC mass concentrations for the background sites (Welgegund, Louis Trichardt, Skukuza, Botsalano) and sites influenced by industrial activities and/or nearby settlements (Elandsfontein, Marikana, Vaal Triangle and Amersfoort) ranged between 0.7 and 1.1, and 1.3 and 1.4 μg m-3, respectively. Similar seasonal patterns were observed at all three sites where continuous measurement data were collected (Elandsfontein, Marikana and Welgegund), with the highest eBC mass concentrations measured from June to October, indicating contributions from household combustion in the cold winter months (June-August), as well as savannah and grassland fires during the dry season (May to mid-October). Diurnal patterns of eBC at Elandsfontein, Marikana and Welgegund indicated maximum concentrations in the early mornings and late evenings, and minima during daytime. From the patterns it could be deduced that for Marikana and Welgegund, household combustion, as well as savannah and grassland fires, were the most significant sources, respectively. Possible contributing sources were explored in greater detail for Elandsfontein, with five main sources being identified as coal-fired power stations, pyrometallurgical smelters, traffic, household combustion, as well as savannah and grassland fires. Industries on the Mpumalanga Highveld are often blamed for all forms of pollution, due to the NO2 hotspot over this area that is attributed to NOx emissions from industries and vehicle emissions from the Johannesburg. Pretoria megacity. However, a comparison of source strengths indicated that household combustion as well as savannah and grassland fires were the most significant sources of eBC, particularly during winter and spring months, while coal-fired power stations, pyrometallurgical smelters and traffic contribute to eBC mass concentration levels year round.
- ItemTracing the Snowball bifurcation of aquaplanets through time reveals a fundamental shift in critical-state dynamics(Göttingen : Copernicus, 2023) Feulner, Georg; Bukenberger, Mona; Petri, StefanThe instability with respect to global glaciation is a fundamental property of the climate system caused by the positive ice-albedo feedback. The atmospheric concentration of carbon dioxide (CO2) at which this Snowball bifurcation occurs changes through Earth's history, most notably because of the slowly increasing solar luminosity. Quantifying this critical CO2 concentration is not only interesting from a climate dynamics perspective but also constitutes an important prerequisite for understanding past Snowball Earth episodes, as well as the conditions for habitability on Earth and other planets. Earlier studies are limited to investigations with very simple climate models for Earth's entire history or studies of individual time slices carried out with a variety of more complex models and for different boundary conditions, making comparisons and the identification of secular changes difficult. Here, we use a coupled climate model of intermediate complexity to trace the Snowball bifurcation of an aquaplanet through Earth's history in one consistent model framework. We find that the critical CO2 concentration decreased more or less logarithmically with increasing solar luminosity until about 1 billion years ago but dropped faster in more recent times. Furthermore, there was a fundamental shift in the dynamics of the critical state about 1.2 billion years ago (unrelated to the downturn in critical CO2 values), driven by the interplay of wind-driven sea-ice dynamics and the surface energy balance: for critical states at low solar luminosities, the ice line lies in the Ferrel cell, stabilised by the poleward winds despite moderate meridional temperature gradients under strong greenhouse warming. For critical states at high solar luminosities, on the other hand, the ice line rests at the Hadley cell boundary, stabilised against the equatorward winds by steep meridional temperature gradients resulting from the increased solar energy input at lower latitudes and stronger Ekman transport in the ocean.
- ItemHighly active and selective photochemical reduction of CO2 to CO using molecular-defined cyclopentadienone iron complexes(Cambridge : Soc., 2015) Rosas-Hernández, Alonso; Alsabeh, Pamela G.; Barsch, Enrico; Junge, Hernrik; Ludwig, Ralf; Beller, MatthiasHerein, we report highly active (cyclopentadienone)iron–tricarbonyl complexes for CO2 photoreduction using visible light with an Ir complex as photosensitizer and TEOA as electron/proton donor. Turnover numbers (TON) of ca. 600 (1 h) with initial turnover frequencies (TOF) up to 22.2 min−1 were observed. Operando FTIR measurements allowed for the proposal of a plausible mechanism for catalyst activation.
- ItemTowards a methanol economy based on homogeneous catalysis: methanol to H2 and CO2 to methanol(Cambridge : Soc., 2015) Alberico, E.; Nielsen, M.The possibility to implement both the exhaustive dehydrogenation of aqueous methanol to hydrogen and CO2 and the reverse reaction, the hydrogenation of CO2 to methanol and water, may pave the way to a methanol based economy as part of a promising renewable energy system. Recently, homogeneous catalytic systems have been reported which are able to promote either one or the other of the two reactions under mild conditions. Here, we review and discuss these developments.
- ItemKey knowledge and data gaps in modelling the influence of CO2 concentration on the terrestrial carbon sink(München : Elsevier, 2016) Pugh, T.A.M.; Müller, C.; Arneth, A.; Haverd, V.; Smith, B.Primary productivity of terrestrial vegetation is expected to increase under the influence of increasing atmospheric carbon dioxide concentrations ([CO2]). Depending on the fate of such additionally fixed carbon, this could lead to an increase in terrestrial carbon storage, and thus a net terrestrial sink of atmospheric carbon. Such a mechanism is generally believed to be the primary global driver behind the observed large net uptake of anthropogenic CO2 emissions by the biosphere. Mechanisms driving CO2 uptake in the Terrestrial Biosphere Models (TBMs) used to attribute and project terrestrial carbon sinks, including that from increased [CO2], remain in large parts unchanged since those models were conceived two decades ago. However, there exists a large body of new data and understanding providing an opportunity to update these models, and directing towards important topics for further research. In this review we highlight recent developments in understanding of the effects of elevated [CO2] on photosynthesis, and in particular on the fate of additionally fixed carbon within the plant with its implications for carbon turnover rates, on the regulation of photosynthesis in response to environmental limitations on in-plant carbon sinks, and on emergent ecosystem responses. We recommend possible avenues for model improvement and identify requirements for better data on core processes relevant to the understanding and modelling of the effect of increasing [CO2] on the global terrestrial carbon sink.
- ItemThe GGCMI Phase 2 experiment: Global gridded crop model simulations under uniform changes in CO2, temperature, water, and nitrogen levels (protocol version 1.0)(Katlenburg-Lindau : Copernicus, 2020) Franke, James A.; Müller, Christoph; Elliott, Joshua; Ruane, Alex C.; Jägermeyr, Jonas; Balkovic, Juraj; Ciais, Philippe; Dury, Marie; Falloon, Pete D.; Folberth, Christian; François, Louis; Hank, Tobias; Hoffmann, Munir; Izaurralde, R. Cesar; Jacquemin, Ingrid; Jones, Curtis; Khabarov, Nikolay; Koch, Marian; Li, Michelle; Liu, Wenfeng; Olin, Stefan; Phillips, Meridel; Pugh, Thomas A. M.; Reddy, Ashwan; Wang, Xuhui; Williams, Karina; Zabel, Florian; Moyer, Elisabeth J.Concerns about food security under climate change motivate efforts to better understand future changes in crop yields. Process-based crop models, which represent plant physiological and soil processes, are necessary tools for this purpose since they allow representing future climate and management conditions not sampled in the historical record and new locations to which cultivation may shift. However, process-based crop models differ in many critical details, and their responses to different interacting factors remain only poorly understood. The Global Gridded Crop Model Intercomparison (GGCMI) Phase 2 experiment, an activity of the Agricultural Model Intercomparison and Improvement Project (AgMIP), is designed to provide a systematic parameter sweep focused on climate change factors and their interaction with overall soil fertility, to allow both evaluating model behavior and emulating model responses in impact assessment tools. In this paper we describe the GGCMI Phase 2 experimental protocol and its simulation data archive. A total of 12 crop models simulate five crops with systematic uniform perturbations of historical climate, varying CO2, temperature, water supply, and applied nitrogen (“CTWN”) for rainfed and irrigated agriculture, and a second set of simulations represents a type of adaptation by allowing the adjustment of growing season length. We present some crop yield results to illustrate general characteristics of the simulations and potential uses of the GGCMI Phase 2 archive. For example, in cases without adaptation, modeled yields show robust decreases to warmer temperatures in almost all regions, with a nonlinear dependence that means yields in warmer baseline locations have greater temperature sensitivity. Inter-model uncertainty is qualitatively similar across all the four input dimensions but is largest in high-latitude regions where crops may be grown in the future.