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- ItemEffects of aerosol size and coating thickness on the molecular detection using extractive electrospray ionization(Katlenburg-Lindau : European Geosciences Union, 2021) Lee, Chuan Ping; Surdu, Mihnea; Bell, David M.; Lamkaddam, Houssni; Wang, Mingyi; Ataei, Farnoush; Hofbauer, Victoria; Lopez, Brandon; Donahue, Neil M.; Dommen, Josef; Prevot, Andre S. H.; Slowik, Jay G.; Wang, Dongyu; Baltensperger, Urs; El Haddad, ImadExtractive electrospray ionization (EESI) has been a well-known technique for high-throughput online molecular characterization of chemical reaction products and intermediates, detection of native biomolecules, in vivo metabolomics, and environmental monitoring with negligible thermal and ionization-induced fragmentation for over two decades. However, the EESI extraction mechanism remains uncertain. Prior studies disagree on whether particles between 20 and 400nm diameter are fully extracted or if the extraction is limited to the surface layer. Here, we examined the analyte extraction mechanism by assessing the influence of particle size and coating thickness on the detection of the molecules therein. We find that particles are extracted fully: organics-coated NH4NO3 particles with a fixed core volume (156 and 226nm in diameter without coating) showed constant EESI signals for NH4NO3 independent of the shell coating thickness, while the signals of the secondary organic molecules comprising the shell varied proportionally to the shell volume. We also found that the EESI sensitivity exhibited a strong size dependence, with an increase in sensitivity by 1-3 orders of magnitude as particle size decreased from 300 to 30nm. This dependence varied with the electrospray (ES) droplet size, the particle size and the residence time for coagulation in the EESI inlet, suggesting that the EESI sensitivity was influenced by the coagulation coefficient between particles and ES droplets. Overall, our results indicate that, in the EESI, particles are fully extracted by the ES droplets regardless of the chemical composition, when they are collected by the ES droplets. However, their coalescence is not complete and depends strongly on their size. This size dependence is especially relevant when EESI is used to probe size-varying particles as is the case in aerosol formation and growth studies with size ranges below 100nm. © 2021 The Author(s).
- ItemA generic pixel-to-point comparison for simulated large-scale ecosystem properties and ground-based observations: An example from the Amazon region(Katlenburg-Lindau : Copernicus, 2018) Rammig, Anja; Heinke, Jens; Hofhansl, Florian; Verbeeck, Hans; Baker, Timothy R.; Christoffersen, Bradley; Ciais, Philippe; De Deurwaerder, Hannes; Fleischer, Katrin; Galbraith, David; Guimberteau, Matthieu; Huth, Andreas; Johnson, Michelle; Krujit, Bart; Langerwisch, Fanny; Meir, Patrick; Papastefanou, Phillip; Sampaio, Gilvan; Thonicke, Kirsten; von Randow, Celso; Zang, Christian; Rödig, EdnaComparing model output and observed data is an important step for assessing model performance and quality of simulation results. However, such comparisons are often hampered by differences in spatial scales between local point observations and large-scale simulations of grid cells or pixels. In this study, we propose a generic approach for a pixel-to-point comparison and provide statistical measures accounting for the uncertainty resulting from landscape variability and measurement errors in ecosystem variables. The basic concept of our approach is to determine the statistical properties of small-scale (within-pixel) variability and observational errors, and to use this information to correct for their effect when large-scale area averages (pixel) are compared to small-scale point estimates. We demonstrate our approach by comparing simulated values of aboveground biomass, woody productivity (woody net primary productivity, NPP) and residence time of woody biomass from four dynamic global vegetation models (DGVMs) with measured inventory data from permanent plots in the Amazon rainforest, a region with the typical problem of low data availability, potential scale mismatch and thus high model uncertainty. We find that the DGVMs under- and overestimate aboveground biomass by 25% and up to 60%, respectively. Our comparison metrics provide a quantitative measure for model-data agreement and show moderate to good agreement with the region-wide spatial biomass pattern detected by plot observations. However, all four DGVMs overestimate woody productivity and underestimate residence time of woody biomass even when accounting for the large uncertainty range of the observational data. This is because DGVMs do not represent the relation between productivity and residence time of woody biomass correctly. Thus, the DGVMs may simulate the correct large-scale patterns of biomass but for the wrong reasons. We conclude that more information about the underlying processes driving biomass distribution are necessary to improve DGVMs. Our approach provides robust statistical measures for any pixel-to-point comparison, which is applicable for evaluation of models and remote-sensing products.
- ItemInvestigation of the Effects of Torrefaction Temperature and Residence Time on the Fuel Quality of Corncobs in a Fixed-Bed Reactor(Basel : MDPI, 2022) Orisaleye, Joseph I.; Jekayinfa, Simeon O.; Pecenka, Ralf; Ogundare, Adebayo A.; Akinseloyin, Michael O.; Fadipe, Opeyemi L.Biomass from agriculture is a promising alternative fuel due to its carbon-neutral feature. However, raw biomass does not have properties required for its direct utilization for energy generation. Torrefaction is considered as a pretreatment method to improve the properties of biomass for energy applications. This study was aimed at investigating the effects of torrefaction temperature and residence time on some physical and chemical properties of torrefied corncobs. Therefore, a fixed-bed torrefaction reactor was developed and used in the torrefaction of corncobs. The torrefaction process parameters investigated were the torrefaction temperature (200, 240, and 280 °C) and the residence time (30, 60, and 90 min). The effects of these parameters on the mass loss, grindability, chemical composition, and calorific value of biomass were investigated. It was shown that the mass loss increased with increasing torrefaction temperature and residence time. The grinding throughput of the biomass was improved by increasing both the torrefaction temperature and the residence time. Torrefaction at higher temperatures and longer residence times had greater effects on the reduction in particle size of the milled corncobs. The calorific value was highest at a torrefaction temperature of 280 °C and a residence time of 90 min. The energy yield for all treatments ranged between 92.8 and 99.2%. The results obtained in this study could be useful in the operation and design of torrefaction reactors. They also provided insight into parameters to be investigated for optimization of the torrefaction reactor.
- ItemThe Earth system model CLIMBER-X v1.0 - Part 2: The global carbon cycle(Katlenburg-Lindau : Copernicus, 2023) Willeit, Matteo; Ilyina, Tatiana; Liu, Bo; Heinze, Christoph; Perrette, Mahé; Heinemann, Malte; Dalmonech, Daniela; Brovkin, Victor; Munhoven, Guy; Börker, Janine; Hartmann, Jens; Romero-Mujalli, Gibran; Ganopolski, AndreyThe carbon cycle component of the newly developed Earth system model of intermediate complexity CLIMBER-X is presented. The model represents the cycling of carbon through the atmosphere, vegetation, soils, seawater and marine sediments. Exchanges of carbon with geological reservoirs occur through sediment burial, rock weathering and volcanic degassing. The state-of-the-art HAMOCC6 model is employed to simulate ocean biogeochemistry and marine sediment processes. The land model PALADYN simulates the processes related to vegetation and soil carbon dynamics, including permafrost and peatlands. The dust cycle in the model allows for an interactive determination of the input of the micro-nutrient iron into the ocean. A rock weathering scheme is implemented in the model, with the weathering rate depending on lithology, runoff and soil temperature. CLIMBER-X includes a simple representation of the methane cycle, with explicitly modelled natural emissions from land and the assumption of a constant residence time of CH4 in the atmosphere. Carbon isotopes 13C and 14C are tracked through all model compartments and provide a useful diagnostic for model-data comparison. A comprehensive evaluation of the model performance for the present day and the historical period shows that CLIMBER-X is capable of realistically reproducing the historical evolution of atmospheric CO2 and CH4 but also the spatial distribution of carbon on land and the 3D structure of biogeochemical ocean tracers. The analysis of model performance is complemented by an assessment of carbon cycle feedbacks and model sensitivities compared to state-of-the-art Coupled Model Intercomparison Project Phase 6 (CMIP6) models. Enabling an interactive carbon cycle in CLIMBER-X results in a relatively minor slow-down of model computational performance by ∼ 20 % compared to a throughput of ∼ 10 000 simulation years per day on a single node with 16 CPUs on a high-performance computer in a climate-only model set-up. CLIMBER-X is therefore well suited to investigating the feedbacks between climate and the carbon cycle on temporal scales ranging from decades to >100000 years.