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Ecosystems play a pivotal role in addressing climate change but are also highly susceptible to drastic environmental changes. Investigating their historical dynamics can enhance our understanding of how they might respond to unprecedented future environmental shifts. With Arctic lakes currently under substantial pressure from climate change, lessons from the past can guide our understanding of potential disruptions to these lakes. However, individual lake systems are multifaceted and complex. Traditional isolated lake studies often fail to provide a global perspective because localized nuances—like individual lake parameters, catchment areas, and lake histories—can overshadow broader conclusions. In light of these complexities, a more nuanced approach is essential to analyze lake systems in a global context.
A key to addressing this challenge lies in the data-driven analysis of sedimentological records from various northern lake systems. This dissertation emphasizes lake systems in the northern Eurasian region, particularly in Russia (n=59). For this doctoral thesis, we collected sedimentological data from various sources, which required a standardized framework for further analysis. Therefore, we designed a conceptual model for integrating and standardizing heterogeneous multi-proxy data into a relational database management system (PostgreSQL). Creating a database from the collected data enabled comparative numerical analyses between spatially separated lakes as well as between different proxies.
When analyzing numerous lakes, establishing a common frame of reference was crucial. We achieved this by converting proxy values from depth dependency to age dependency. This required consistent age calculations across all lakes and proxies using one age-depth modeling software. Recognizing the broader implications and potential pitfalls of this, we developed the LANDO approach ("Linked Age and Depth Modelling"). LANDO is an innovative integration of multiple age-depth modeling software into a singular, cohesive platform (Jupyter Notebook). Beyond its ability to aggregate data from five renowned age-depth modeling software, LANDO uniquely empowers users to filter out implausible model outcomes using robust geoscientific data. Our method is not only novel but also significantly enhances the accuracy and reliability of lake analyses.
Considering the preceding steps, this doctoral thesis further examines the relationship between carbon in sediments and temperature over the last 21,000 years. Initially, we hypothesized a positive correlation between carbon accumulation in lakes and modelled paleotemperature. Our homogenized dataset from heterogeneous lakes confirmed this association, even if the highest temperatures throughout our observation period do not correlate with the highest carbon values. We assume that rapid warming events contribute more to high accumulation, while sustained warming leads to carbon outgassing. Considering the current high concentration of carbon in the atmosphere and rising temperatures, ongoing climate change could cause northern lake systems to contribute to a further increase in atmospheric carbon (positive feedback loop). While our findings underscore the reliability of both our standardized data and the LANDO method, expanding our dataset might offer even greater assurance in our conclusions.
With Arctic ground as a huge and temperature-sensitive carbon reservoir, maintaining low ground temperatures and frozen conditions to prevent further carbon emissions that contrib-ute to global climate warming is a key element in humankind’s fight to maintain habitable con-ditions on earth. Former studies showed that during the late Pleistocene, Arctic ground condi-tions were generally colder and more stable as the result of an ecosystem dominated by large herbivorous mammals and vast extents of graminoid vegetation – the mammoth steppe. Characterised by high plant productivity (grassland) and low ground insulation due to animal-caused compression and removal of snow, this ecosystem enabled deep permafrost aggrad-ation. Now, with tundra and shrub vegetation common in the terrestrial Arctic, these effects are not in place anymore. However, it appears to be possible to recreate this ecosystem local-ly by artificially increasing animal numbers, and hence keep Arctic ground cold to reduce or-ganic matter decomposition and carbon release into the atmosphere.
By measuring thaw depth, total organic carbon and total nitrogen content, stable carbon iso-tope ratio, radiocarbon age, n-alkane and alcohol characteristics and assessing dominant vegetation types along grazing intensity transects in two contrasting Arctic areas, it was found that recreating conditions locally, similar to the mammoth steppe, seems to be possible. For permafrost-affected soil, it was shown that intensive grazing in direct comparison to non-grazed areas reduces active layer depth and leads to higher TOC contents in the active layer soil. For soil only frozen on top in winter, an increase of TOC with grazing intensity could not be found, most likely because of confounding factors such as vertical water and carbon movement, which is not possible with an impermeable layer in permafrost. In both areas, high animal activity led to a vegetation transformation towards species-poor graminoid-dominated landscapes with less shrubs. Lipid biomarker analysis revealed that, even though the available organic material is different between the study areas, in both permafrost-affected and sea-sonally frozen soils the organic material in sites affected by high animal activity was less de-composed than under less intensive grazing pressure. In conclusion, high animal activity af-fects decomposition processes in Arctic soils and the ground thermal regime, visible from reduced active layer depth in permafrost areas. Therefore, grazing management might be utilised to locally stabilise permafrost and reduce Arctic carbon emissions in the future, but is likely not scalable to the entire permafrost region.
The reliance on fossil fuels has resulted in an abnormal increase in the concentration of greenhouse gases, contributing to the global climate crisis. In response, a rapid transition to renewable energy sources has begun, particularly lithium-ion batteries, playing a crucial role in the green energy transformation. However, concerns regarding the availability and geopolitical implications of lithium have prompted the exploration of alternative rechargeable battery systems, such as sodium-ion batteries. Sodium is significantly abundant and more homogeneously distributed in the crust and seawater, making it easier and less expensive to extract than lithium. However, because of the mysterious nature of its components, sodium-ion batteries are not yet sufficiently advanced to take the place of lithium-ion batteries. Specifically, sodium exhibits a more metallic character and a larger ionic radius, resulting in a different ion storage mechanism utilized in lithium-ion batteries. Innovations in synthetic methods, post-treatments, and interface engineering clearly demonstrate the significance of developing high-performance carbonaceous anode materials for sodium-ion batteries. The objective of this dissertation is to present a systematic approach for fabricating efficient, high-performance, and sustainable carbonaceous anode materials for sodium-ion batteries. This will involve a comprehensive investigation of different chemical environments and post-modification techniques as well.
This dissertation focuses on three main objectives. Firstly, it explores the significance of post-synthetic methods in designing interfaces. A conformal carbon nitride coating is deposited through chemical vapor deposition on a carbon electrode as an artificial solid-electrolyte interface layer, resulting in improved electrochemical performance. The interaction between the carbon nitride artificial interface and the carbon electrode enhances initial Coulombic efficiency, rate performance, and total capacity. Secondly, a novel process for preparing sulfur-rich carbon as a high-performing anode material for sodium-ion batteries is presented. The method involves using an oligo-3,4-ethylenedioxythiophene precursor for high sulfur content hard carbon anode to investigate the sulfur heteroatom effect on the electrochemical sodium storage mechanism. By optimizing the condensation temperature, a significant transformation in the materials’ nanostructure is achieved, leading to improved electrochemical performance. The use of in-operando small-angle X-ray scattering provides valuable insights into the interaction between micropores and sodium ions during the electrochemical processes. Lastly, the development of high-capacity hard carbon, derived from 5-hydroxymethyl furfural, is examined. This carbon material exhibits exceptional performance at both low and high current densities. Extensive electrochemical and physicochemical characterizations shed light on the sodium storage mechanism concerning the chemical environment, establishing the material’s stability and potential applications in sodium-ion batteries.
This study, based on new and high quality in situ observations, quantifies for the first time, the individual contributions of light-absorbing aerosols (black carbon (BC), brown carbon (BrC) and dust) to aerosol absorption over the Indo-Gangetic Plain (IGP) and the Himalayan foothill region, a relatively poorly studied region with several sensitive ecosystems of global importance, as well as highly vulnerable populations. The annual and seasonal average single scattering albedo (SSA) over Kathmandu is the lowest of all the locations. The SSA over Kathmandu is < 0.89 during all seasons, which confirms the dominance of light-absorbing carbonaceous aerosols from local and regional sources over Kathmandu. It is observed here that the SSA decreases with increasing elevation, confirming the dominance of light absorbing carbonaceous aerosols at higher elevations. In contrast, the SSA over the IGP does not exhibit a pronounced spatial variation. BC dominates (>= 75%) the aerosol absorption over the IGP and the Himalayan foothills throughout the year. Higher BC concentration at elevated locations in the Himalayas leads to lower SSA at elevated locations in the Himalayas. The contribution of dust to aerosol absorption is higher throughout the year over the IGP than over the Himalayan foothills. The aerosol absorption over South Asia is very high, exceeding available observations over East Asia, and also exceeds previous model estimates. This quantification will be valuable as observational constraints to help improve regional simulations of climate change, impacts on the glaciers and the hydrological cycle, and will help to direct the focus towards BC as the main contributor to aerosol-induced warming in the region.
In flowering plants, sugars act as carbon sources providing energy for developing embryos and seeds. Although most studies focus on carbon metabolism in whole seeds, knowledge about how particular sugars contribute to the developmental transitions during embryogenesis is scarce. To develop a quantitative understanding of how carbon composition changes during embryo development, and to determine how sugar status contributes to final seed or embryo size, we performed metabolic profiling of hand-dissected embryos at late torpedo and mature stages, and dormant seeds, in two Arabidopsis thaliana accessions with medium [Columbia-0 (Col-0)] and large [Burren-0 (Bur-0)] seed sizes, respectively. Our results show that, in both accessions, metabolite profiles of embryos largely differ from those of dormant seeds. We found that developmental transitions from torpedo to mature embryos, and further to dormant seeds, are associated with major metabolic switches in carbon reserve accumulation. While glucose, sucrose, and starch predominantly accumulated during seed dormancy, fructose levels were strongly elevated in mature embryos. Interestingly, Bur-0 seeds contain larger mature embryos than Col-0 seeds. Fructose and starch were accumulated to significantly higher levels in mature Bur-0 than Col-0 embryos, suggesting that they contribute to the enlarged mature Bur-0 embryos. Furthermore, we found that Bur-0 embryos accumulated a higher level of sucrose compared to hexose sugars and that changes in sucrose metabolism are mediated by sucrose synthase (SUS), with SUS genes acting non-redundantly, and in a tissue-specific manner to utilize sucrose during late embryogenesis.
To achieve a sustainable energy economy, it is necessary to turn back on the combustion of fossil fuels as a means of energy production and switch to renewable sources. However, their temporal availability does not match societal consumption needs, meaning that renewably generated energy must be stored in its main generation times and allocated during peak consumption periods. Electrochemical energy storage (EES) in general is well suited due to its infrastructural independence and scalability. The lithium ion battery (LIB) takes a special place, among EES systems due to its energy density and efficiency, but the scarcity and uneven geological occurrence of minerals and ores vital for many cell components, and hence the high and fluctuating costs will decelerate its further distribution.
The sodium ion battery (SIB) is a promising successor to LIB technology, as the fundamental setup and cell chemistry is similar in the two systems. Yet, the most widespread negative electrode material in LIBs, graphite, cannot be used in SIBs, as it cannot store sufficient amounts of sodium at reasonable potentials. Hence, another carbon allotrope, non-graphitizing or hard carbon (HC) is used in SIBs. This material consists of turbostratically disordered, curved graphene layers, forming regions of graphitic stacking and zones of deviating layers, so-called internal or closed pores.
The structural features of HC have a substantial impact of the charge-potential curve exhibited by the carbon when it is used as the negative electrode in an SIB. At defects and edges an adsorption-like mechanism of sodium storage is prevalent, causing a sloping voltage curve, ill-suited for the practical application in SIBs, whereas a constant voltage plateau of relatively high capacities is found immediately after the sloping region, which recent research attributed to the deposition of quasimetallic sodium into the closed pores of HC.
Literature on the general mechanism of sodium storage in HCs and especially the role of the closed pore is abundant, but the influence of the pore geometry and chemical nature of the HC on the low-potential sodium deposition is yet in an early stage. Therefore, the scope of this thesis is to investigate these relationships using suitable synthetic and characterization methods. Materials of precisely known morphology, porosity, and chemical structure are prepared in clear distinction to commonly obtained ones and their impact on the sodium storage characteristics is observed. Electrochemical impedance spectroscopy in combination with distribution of relaxation times analysis is further established as a technique to study the sodium storage process, in addition to classical direct current techniques, and an equivalent circuit model is proposed to qualitatively describe the HC sodiation mechanism, based on the recorded data. The obtained knowledge is used to develop a method for the preparation of closed porous and non-porous materials from open porous ones, proving not only the necessity of closed pores for efficient sodium storage, but also providing a method for effective pore closure and hence the increase of the sodium storage capacity and efficiency of carbon materials.
The insights obtained and methods developed within this work hence not only contribute to the better understanding of the sodium storage mechanism in carbon materials of SIBs, but can also serve as guidance for the design of efficient electrode materials.
Ice-wedge polygons are widespread periglacial features and influence landscape hydrology and carbon storage. The influence of climate and topography on polygon development is not entirely clear, however, giving high uncertainties to projections of permafrost development. We studied the mid- to late Holocene development of modern ice-wedge polygon sites to explore drivers of change and reasons for long-term stability. We analyzed organic carbon, total nitrogen, stable carbon isotopes, grain size composition and plant macrofossils in six cores from three polygons. We found that ail sites developed from aquatic to wetland conditions. In the mid-Holocene, shallow lakes and partly submerged ice-wedge polygons existed at the studied sites. An erosional hiatus of ca 5000 years followed, and ice-wedge polygons re-initiated within the last millennium. Ice-wedge melt and surface drying during the last century were linked to climatic warming. The influence of climate on ice-wedge polygon development was outweighed by geomorphology during most of the late Holocene. Recent warming, however, caused ice-wedge degradation at all sites. Our study showed that where waterlogged ground was maintained, low-centered polygons persisted for millennia. Ice-wedge melt and increased drainage through geomorphic disturbance, however, triggered conversion into high-centered polygons and may lead to self-enhancing degradation under continued warming.
Glacial-interglacial variations in CO2 and methane in polar ice cores have been attributed, in part, to changes in global wetland extent, but the wetland distribution before the Last Glacial Maximum (LGM, 21 ka to 18 ka) remains virtually unknown. We present a study of global peatland extent and carbon (C) stocks through the last glacial cycle (130 ka to present) using a newly compiled database of 1,063 detailed stratigraphic records of peat deposits buried by mineral sediments, as well as a global peatland model. Quantitative agreement between modeling and observations shows extensive peat accumulation before the LGM in northern latitudes (> 40 degrees N), particularly during warmer periods including the last interglacial (130 ka to 116 ka, MIS 5e) and the interstadial (57 ka to 29 ka, MIS 3). During cooling periods of glacial advance and permafrost formation, the burial of northern peatlands by glaciers and mineral sediments decreased active peatland extent, thickness, and modeled C stocks by 70 to 90% from warmer times. Tropical peatland extent and C stocks show little temporal variation throughout the study period. While the increased burial of northern peats was correlated with cooling periods, the burial of tropical peat was predominately driven by changes in sea level and regional hydrology. Peat burial by mineral sediments represents a mechanism for long-term terrestrial C storage in the Earth system. These results show that northern peatlands accumulate significant C stocks during warmer times, indicating their potential for C sequestration during the warming Anthropocene.
MoS2, a typical layered transition-metal dichalcogenide, is promising as an electrode material in supercapacitors. However, its low electrical conductivity could lead to limited capacitance if applied in electrochemical devices. Herein, a new nanostructure composed of hollow carbon-MoS2-carbon was successfully synthesized through an L-cysteine-assisted hydrothermal method by using gibbsite as a template and polydopamine as a carbon precursor. After calcination and etching of the gibbsite template, uniform hollow platelets, which were made of a sandwich-like assembly of partial graphitic carbon and two-dimensional layered MoS2 flakes, were obtained. The platelets showed excellent dispersibility and stability in water, and good electrical conductivity due to carbon provided by the calcination of polydopamine coatings. The hollow nanoplate morphology of the material provided a high specific surface area of 543 m(2) g(-1), a total pore volume of 0.677 cm(3) g(-1), and fairly small mesopores (approximate to 5.3 nm). The material was applied in a symmetric supercapacitor and exhibited a specific capacitance of 248 F g(-1) (0.12 F cm(-2)) at a constant current density of 0.1 Ag-1; thus suggesting that hollow carbon-MoS2 carbon nanoplates are promising candidate materials for supercapacitors.
Permafrost thaw subjects previously frozen organic carbon (OC) to microbial decomposition, generating the greenhouse gases (GHG) carbon dioxide (CO2) and methane (CH4) and fueling a positive climate feedback. Over one quarter of permafrost OC is stored in deep, ice-rich Pleistocene-aged yedoma permafrost deposits. We used a combination of anaerobic incubations, microbial sequencing, and ultrahigh-resolution mass spectrometry to show yedoma OC biolability increases with depth along a 12-m yedoma profile. In incubations at 3 degrees C and 13 degrees C, GHG production per unit OC at 12-versus 1.3-m depth was 4.6 and 20.5 times greater, respectively. Bacterial diversity decreased with depth and we detected methanogens at all our sampled depths, suggesting that in situ microbial communities are equipped to metabolize thawed OC into CH4. We concurrently observed an increase in the relative abundance of reduced, saturated OC compounds, which corresponded to high proportions of C mineralization and positively correlated with anaerobic GHG production potentials and higher proportions of OC being mineralized as CH4. Taking into account the higher global warming potential (GWP) of CH4 compared to CO2, thawed yedoma sediments in our study had 2 times higher GWP at 12-versus 9.0-m depth at 3 degrees C and 15 times higher GWP at 13 degrees C. Considering that yedoma is vulnerable to processes that thaw deep OC, our findings imply that it is important to account for this increasing GHG production and GWP with depth to better understand the disproportionate impact of yedoma on the magnitude of the permafrost carbon feedback.