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- ItemCurrent Advances in TiO2-Based Nanostructure Electrodes for High Performance Lithium Ion Batteries(Basel : MDPI, 2018-2-6) Madian, Mahmoud; Eychmüller, Alexander; Giebeler, LarsThe lithium ion battery (LIB) has proven to be a very reliably used system to store electrical energy, for either mobile or stationary applications. Among others, TiO2-based anodes are the most attractive candidates for building safe and durable lithium ion batteries with high energy density. A variety of TiO2 nanostructures has been thoroughly investigated as anodes in LIBs, e.g., nanoparticles, nanorods, nanoneedles, nanowires, and nanotubes discussed either in their pure form or in composites. In this review, we present the recent developments and breakthroughs demonstrated to synthesize safe, high power, and low cost nanostructured titania-based anodes. The reader is provided with an in-depth review of well-oriented TiO2-based nanotubes fabricated by anodic oxidation. Other strategies for modification of TiO2-based anodes with other elements or materials are also highlighted in this report.
- ItemTextured Sb2Te3 films and GeTe/Sb2Te3 superlattices grown on amorphous substrates by molecular beam epitaxy(New York : American Institute of Physics, 2017) Boschker, Jos E.; Tisbi, E.; Placidi, E.; Momand, Jamo; Redaelli, Andrea; Kooi, Bart J.; Arciprete, Fabrizio; Calarco, RaffaellaThe realization of textured films of 2-dimensionally (2D) bonded materials on amorphous substrates is important for the integration of this material class with silicon based technology. Here, we demonstrate the successful growth by molecular beam epitaxy of textured Sb2Te3 films and GeTe/Sb2Te3 superlattices on two types of amorphous substrates: carbon and SiO2. X-ray diffraction measurements reveal that the out-of-plane alignment of grains in the layers has a mosaic spread with a full width half maximum of 2.8°. We show that a good texture on SiO2 is only obtained for an appropriate surface preparation, which can be performed by ex situ exposure to Ar+ ions or by in situ exposure to an electron beam. X-ray photoelectron spectroscopy reveals that this surface preparation procedure results in reduced oxygen content. Finally, it is observed that film delamination can occur when a capping layer is deposited on top of a superlattice with a good texture. This is attributed to the stress in the capping layer and can be prevented by using optimized deposition conditions of the capping layer. The obtained results are also relevant to the growth of other 2D materials on amorphous substrates.
- ItemModeling forest plantations for carbon uptake with the LPJmL dynamic global vegetation model(Göttingen : Copernicus Publ., 2019) Braakhekke, Maarten C.; Doelman, Jonathan C.; Baas, Peter; Müller, Christoph; Schaphoff, Sibyll; Stehfest, Elke; van Vuuren, Detlef P.We present an extension of the dynamic global vegetation model, Lund-Potsdam-Jena Managed Land (LPJmL), to simulate planted forests intended for carbon (C) sequestration. We implemented three functional types to simulate plantation trees in temperate, tropical, and boreal climates. The parameters of these functional types were optimized to fit target growth curves (TGCs). These curves represent the evolution of stemwood C over time in typical productive plantations and were derived by combining field observations and LPJmL estimates for equivalent natural forests. While the calibrated model underestimates stemwood C growth rates compared to the TGCs, it represents substantial improvement over using natural forests to represent afforestation. Based on a simulation experiment in which we compared global natural forest versus global forest plantation, we found that forest plantations allow for much larger C uptake rates on the timescale of 100 years, with a maximum difference of a factor of 1.9, around 54 years. In subsequent simulations for an ambitious but realistic scenario in which 650Mha (14% of global managed land, 4.5% of global land surface) are converted to forest over 85 years, we found that natural forests take up 37PgC versus 48PgC for forest plantations. Comparing these results to estimations of C sequestration required to achieve the 2°C climate target, we conclude that afforestation can offer a substantial contribution to climate mitigation. Full evaluation of afforestation as a climate change mitigation strategy requires an integrated assessment which considers all relevant aspects, including costs, biodiversity, and trade-offs with other land-use types. Our extended version of LPJmL can contribute to such an assessment by providing improved estimates of C uptake rates by forest plantations. © 2019 American Institute of Physics Inc.. All rights reserved.
- ItemEstimating global cropland production from 1961 to 2010(München : European Geopyhsical Union, 2017) Han, Pengfei; Zeng, Ning; Zhao, Fang; Lin, XiaohuiGlobal cropland net primary production (NPP) has tripled over the last 50 years, contributing 17–45 % to the increase in global atmospheric CO2 seasonal amplitude. Although many regional-scale comparisons have been made between statistical data and modeling results, long-term national comparisons across global croplands are scarce due to the lack of detailed spatiotemporal management data. Here, we conducted a simulation study of global cropland NPP from 1961 to 2010 using a process-based model called Vegetation–Global Atmosphere–Soil (VEGAS) and compared the results with Food and Agriculture Organization of the United Nations (FAO) statistical data on both continental and country scales. According to the FAO data, the global cropland NPP was 1.3, 1.8, 2.2, 2.6, 3.0, and 3.6 PgC yr−1 in the 1960s, 1970s, 1980s, 1990s, 2000s, and 2010s, respectively. The VEGAS model captured these major trends on global and continental scales. The NPP increased most notably in the US Midwest, western Europe, and the North China Plain and increased modestly in Africa and Oceania. However, significant biases remained in some regions such as Africa and Oceania, especially in temporal evolution. This finding is not surprising as VEGAS is the first global carbon cycle model with full parameterization representing the Green Revolution. To improve model performance for different major regions, we modified the default values of management intensity associated with the agricultural Green Revolution differences across various regions to better match the FAO statistical data at the continental level and for selected countries. Across all the selected countries, the updated results reduced the RMSE from 19.0 to 10.5 TgC yr−1 (∼ 45 % decrease). The results suggest that these regional differences in model parameterization are due to differences in socioeconomic development. To better explain the past changes and predict the future trends, it is important to calibrate key parameters on regional scales and develop data sets for land management history.
- ItemQuantifying uncertainties in soil carbon responses to changes in global mean temperature and precipitation(München : European Geopyhsical Union, 2014) Nishina, K.; Ito, A.; Beerling, D.J.; Cadule, P.; Ciais, P.; Clark, D.B.; Friend, A.D.; Kahana, R.; Kato, E.; Keribin, R.; Lucht, W.; Lomas, M.; Rademacher, T.T.; Pavlick, R.; Schaphoff, S.; Vuichard, N.; Warszawaski, L.; Yokohata, T.Soil organic carbon (SOC) is the largest carbon pool in terrestrial ecosystems and may play a key role in biospheric feedbacks with elevated atmospheric carbon dioxide (CO2) in a warmer future world. We examined the simulation results of seven terrestrial biome models when forced with climate projections from four representative-concentration-pathways (RCPs)-based atmospheric concentration scenarios. The goal was to specify calculated uncertainty in global SOC stock projections from global and regional perspectives and give insight to the improvement of SOC-relevant processes in biome models. SOC stocks among the biome models varied from 1090 to 2650 Pg C even in historical periods (ca. 2000). In a higher forcing scenario (i.e., RCP8.5), inconsistent estimates of impact on the total SOC (2099–2000) were obtained from different biome model simulations, ranging from a net sink of 347 Pg C to a net source of 122 Pg C. In all models, the increasing atmospheric CO2 concentration in the RCP8.5 scenario considerably contributed to carbon accumulation in SOC. However, magnitudes varied from 93 to 264 Pg C by the end of the 21st century across biome models. Using the time-series data of total global SOC simulated by each biome model, we analyzed the sensitivity of the global SOC stock to global mean temperature and global precipitation anomalies (ΔT and ΔP respectively) in each biome model using a state-space model. This analysis suggests that ΔT explained global SOC stock changes in most models with a resolution of 1–2 °C, and the magnitude of global SOC decomposition from a 2 °C rise ranged from almost 0 to 3.53 Pg C yr−1 among the biome models. However, ΔP had a negligible impact on change in the global SOC changes. Spatial heterogeneity was evident and inconsistent among the biome models, especially in boreal to arctic regions. Our study reveals considerable climate uncertainty in SOC decomposition responses to climate and CO2 change among biome models. Further research is required to improve our ability to estimate biospheric feedbacks through both SOC-relevant and vegetation-relevant processes.
- ItemAnalytically tractable climate–carbon cycle feedbacks under 21st century anthropogenic forcing(München : European Geopyhsical Union, 2018) Lade, Steven J.; Donges, Jonathan F.; Fetzer, Ingo; Anderies, John M.; Beer, Christian; Cornell, Sarah E.; Gasser, Thomas; Norberg, Jon; Richardson, Katherine; Rockström, Johan; Steffen, WillChanges to climate–carbon cycle feedbacks may significantly affect the Earth system's response to greenhouse gas emissions. These feedbacks are usually analysed from numerical output of complex and arguably opaque Earth system models. Here, we construct a stylised global climate–carbon cycle model, test its output against comprehensive Earth system models, and investigate the strengths of its climate–carbon cycle feedbacks analytically. The analytical expressions we obtain aid understanding of carbon cycle feedbacks and the operation of the carbon cycle. Specific results include that different feedback formalisms measure fundamentally the same climate–carbon cycle processes; temperature dependence of the solubility pump, biological pump, and CO2 solubility all contribute approximately equally to the ocean climate–carbon feedback; and concentration–carbon feedbacks may be more sensitive to future climate change than climate–carbon feedbacks. Simple models such as that developed here also provide "workbenches" for simple but mechanistically based explorations of Earth system processes, such as interactions and feedbacks between the planetary boundaries, that are currently too uncertain to be included in comprehensive Earth system models.
- ItemDeforestation in Amazonia impacts riverine carbon dynamics(München : European Geopyhsical Union, 2016) Langerwisch, Fanny; Walz, Ariane; Rammig, Anja; Tietjen, Britta; Thonicke, Kirsten; Cramer, WolfgangFluxes of organic and inorganic carbon within the Amazon basin are considerably controlled by annual flooding, which triggers the export of terrigenous organic material to the river and ultimately to the Atlantic Ocean. The amount of carbon imported to the river and the further conversion, transport and export of it depend on temperature, atmospheric CO2, terrestrial productivity and carbon storage, as well as discharge. Both terrestrial productivity and discharge are influenced by climate and land use change. The coupled LPJmL and RivCM model system (Langerwisch et al., 2016) has been applied to assess the combined impacts of climate and land use change on the Amazon riverine carbon dynamics. Vegetation dynamics (in LPJmL) as well as export and conversion of terrigenous carbon to and within the river (RivCM) are included. The model system has been applied for the years 1901 to 2099 under two deforestation scenarios and with climate forcing of three SRES emission scenarios, each for five climate models. We find that high deforestation (business-as-usual scenario) will strongly decrease (locally by up to 90%) riverine particulate and dissolved organic carbon amount until the end of the current century. At the same time, increase in discharge leaves net carbon transport during the first decades of the century roughly unchanged only if a sufficient area is still forested. After 2050 the amount of transported carbon will decrease drastically. In contrast to that, increased temperature and atmospheric CO2 concentration determine the amount of riverine inorganic carbon stored in the Amazon basin. Higher atmospheric CO2 concentrations increase riverine inorganic carbon amount by up to 20% (SRES A2). The changes in riverine carbon fluxes have direct effects on carbon export, either to the atmosphere via outgassing or to the Atlantic Ocean via discharge. The outgassed carbon will increase slightly in the Amazon basin, but can be regionally reduced by up to 60% due to deforestation. The discharge of organic carbon to the ocean will be reduced by about 40% under the most severe deforestation and climate change scenario. These changes would have local and regional consequences on the carbon balance and habitat characteristics in the Amazon basin itself as well as in the adjacent Atlantic Ocean.
- ItemEffect of synthesis catalyst on structure of nitrogen-doped carbon nanotubes and electrical conductivity and electromagnetic interference shielding of their polymeric nanocomposites(New York, NY [u.a.] : Pergamon Press, 2016) Arjmand, Mohammad; Chizari, Kambiz; Krause, Beate; Pötschke, Petra; Sundararaj, UttandaramanDifferent catalysts including Co, Fe, and Ni were used to synthesize nitrogen-doped carbon nanotubes (N-CNTs) by chemical vapor deposition technique. Synthesized N-CNTs were melt mixed with a polyvinylidene fluoride (PVDF) matrix using a small scale mixer at different concentrations ranging from 0.3 to 3.5 wt%, and then compression molded. The characterization techniques revealed significant differences in the synthesis yield and the morphological and electrical properties of both N-CNTs and nanocomposites depending on the catalyst type. Whereas Co and Fe resulted in yields comparable to industrial multiwalled CNTs, Ni was much less effective. The N-CNT aspect ratio was the highest for Co catalyst, followed by Ni and Fe, whereas nitrogen content was the highest for Ni. Raman spectroscopy revealed lowest defect number and highest N-CNT crystallinity for Fe catalyst. Characterization of N-CNT/PVDF nanocomposites showed better dispersion for N-CNTs based on Co and Fe as compared to Ni, and the following order of electrical conductivity and electromagnetic interference shielding (from high to low): Co > Fe > Ni. The superior electrical properties of (N-CNT)Co nanocomposites were ascribed to a combination of high synthesis yield, high aspect ratio, low nitrogen content and high crystallinity of N-CNTs combined with a good state of N-CNT dispersion.
- ItemCharacterization of the state of dispersion of carbon nanotubes in polymer nanocomposites(Weinheim : Wiley-VCH Verl., 2011) Buschhorn, Samuel T.; Wichmann, Malte H. G.; Sumfleth, Jan; Schulte, Karl; Pegel, Sven; Kasaliwal, Gaurav R.; Villmow, Tobias; Krause, Beate; Göldel, Andreas; Pötschke, PetraA practical overview of possibilities and limits to characterize the state of dispersion of carbon nanotubes (CNT) in polymer based nanocomposites is given. The most important and widely available methods are discussed with practical employment in mind. One focus is the quantitative characterization of the state of dispersion in solid samples using microscopy techniques such as optical microscopy or transmission electron microscopy. For dispersions of CNTs in aqueous media, solvents or monomers a sedimentation analysis is presented. This way dispersability and dispersion state of CNTs can be assessed. Indirect methods such as electrical conductivity measurements and rheological tests, dynamic differential scanning calorimetry and mechanical test are discussed. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
- ItemA robust iron catalyst for the selective hydrogenation of substituted (iso)quinolones(Cambridge : RSC, 2018) Sahoo, Basudev; Kreyenschulte, Carsten; Agostini, Giovanni; Lund, Henrik; Bachmann, Stephan; Scalone, Michelangelo; Junge, Kathrin; Beller, MatthiasBy applying N-doped carbon modified iron-based catalysts, the controlled hydrogenation of N-heteroarenes, especially (iso)quinolones, is achieved. Crucial for activity is the catalyst preparation by pyrolysis of a carbon-impregnated composite, obtained from iron(ii) acetate and N-aryliminopyridines. As demonstrated by TEM, XRD, XPS and Raman spectroscopy, the synthesized material is composed of Fe(0), Fe3C and FeNx in a N-doped carbon matrix. The decent catalytic activity of this robust and easily recyclable Fe-material allowed for the selective hydrogenation of various (iso)quinoline derivatives, even in the presence of reducible functional groups, such as nitriles, halogens, esters and amides. For a proof-of-concept, this nanostructured catalyst was implemented in the multistep synthesis of natural products and pharmaceutical lead compounds as well as modification of photoluminescent materials. As such this methodology constitutes the first heterogeneous iron-catalyzed hydrogenation of substituted (iso)quinolones with synthetic importance.
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