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Vorwort
(2013)
Sansibar und der Klimawandel
(2013)
We present and discuss the results of crystallographic and electron paramagnetic resonance (EPR) spectroscopic analyses of five tetrachloridocuprate(II) complexes to supply a useful tool for the structural characterisation of the [CuCl4]2− moiety in the liquid state, for example in ionic liquids, or in solution. Bis(benzyltriethylammonium)-, bis(trimethylphenylammonium)-, bis(ethyltriphenylphosphonium)-, bis(benzyltriphenylphosphonium)-, and bis(tetraphenylarsonium)tetrachloridocuprate(II) were synthesised and characterised by elemental, IR, EPR and X-ray analyses. The results of the crystallographic analyses show distorted tetrahedral coordination geometry of all [CuCl4]2− anions in the five complexes and prove that all investigated complexes are stabilised by hydrogen bonds of different intensities. Despite the use of sterically demanding ammonium, phosphonium and arsonium cations to obtain the separation of the paramagnetic Cu(II) centres for EPR spectroscopy no hyperfine structure was observed in the EPR spectra but the principal values of the electron Zeeman tensor, g∥ and g⊥, could be determined. With these EPR data and the crystallographic parameters we were able to carry out a correlation study to anticipate the structural situation of tetrachloridocuprates in different physical states. This correlation is in good agreement with DFT calculations.
Tetrahalidocuprat(II)-komplexe : Untersuchungen zur Relation von Struktur- und EPR-Parametern
(2013)
Films are nanoscopic elements of foams, emulsions, and suspensions that form a paradigm for nanochannel transport that eventually tests the limits of hydrodynamic descriptions. Here, we study the collapse of a freestanding film to its equilibrium. The generation of nanoscale films usually is a slow linear process; using thermal forcing we find unprecedented dynamics with exponentially fast thinning. The complex interplay of thermal convection, interface, and gravitational forces yields optimal turbulent mixing and transport. Domains of collapsed film are generated, elongated, and convected in a beautiful display of chaotic mixing. With a time scale analysis, we identify mixing as the dominant dynamical process responsible for exponential thinning. DOI: 10.1103/PhysRevLett.110.094501
Thin liquid films serve as the paradigms of atmospheric convection, thermal convection in the Earth’s mantle or turbulence in magnetohydrodynamics, thereby connecting with typical systems exhibiting turbulent mixing. In addition, recent research on colloids, interfaces and nanofluids led to advances in the development of micro-mixers (lab-on-a-chip devices). By the thermal forcing of a film, one can reach Rayleigh numbers in the turbulent regime, such that the experiment may serve as a prototype of a mixer on the basis of thermally induced turbulence in free-standing thin liquid films with thicknesses in the nanometer range. Here, the specific experimental results of a setup with a focus on the mixing statistics of a thermally driven two-dimensional thin film are presented. Our setup allows us to capture thin film interference patterns under controlled surface and atmospheric conditions. The convection is realized by placing a cooled copper rod in the center of the film. The temperature gradient between the rod and the atmosphere results in a density gradient in the liquid film, so that the varying buoyancy induces turbulent motion. The flow field is characterized by a newly developed algorithm-color imaging velocimetry (CIV). This analysis determines not only the velocity, but also the full deformation tensor in the Lagrangian frame. On the basis of these insights, the flow in the experiment was investigated with respect to its mixing properties: we calculated the mixing efficiency and entropy of the flow scheme to sufficiently high accuracy.
In den vergangenen Jahren wurden stetig wachsende Produktionskapazitäten von Biokunststoffen aus nachwachsenden Rohstoffe nverzeichnet. Trotz großer Produktionskapazitäten und einem geeigneten Eigenschaftsprofil findet Stärke nur als hydrophile, mit Weichmachern verarbeitete thermoplastische Stärke (TPS) in Form von Blends mit z. B. Polyestern Anwendung. Gleiches gilt für Kunststoffe auf Proteinbasis. Die vorliegende Arbeit hat die Entwicklung von Biokunststoffen auf Stärkebasis zum Ziel, welche ohne externe Weichmacher thermoplastisch verarbeitbar und hydrophob sind sowie ein mechanisches Eigenschaftsprofil aufweisen, welches ein Potenzial zur Herstellung von Materialien für eine Anwendung als Verpackungsmittel bietet. Um die Rohstoffbasis für Biokunststoffe zu erweitern, soll das erarbeitete Konzept auf zwei industriell verfügbare Proteintypen, Zein und Molkenproteinisolat (WPI), übertragen werden. Als geeignete Materialklasse wurden Fettsäureester der Stärke herausgearbeitet. Zunächst fand ein Vergleich der Säurechlorid-Veresterung und der Umesterung von Fettsäurevinylestern statt, woraus letztere als geeignetere Methode hervorging. Durch Variation der Reaktionsparameter konnte diese optimiert und auf eine Serie der Fettsäurevinylester von Butanoat bis Stearat für DS-Werte bis zu 2,2-2,6 angewandt werden. Möglich war somit eine systematische Studie unter Variation der veresterten Fettsäure sowie des Substitutionsgrades (DS). Sämtliche Produkte mit einem DS ab 1,5 wiesen eine ausgprägte Löslichkeit in organischen Lösungsmitteln auf wodurch sowohl die Aufnahme von NMR-Spektren als auch Molmassenbestimmung mittels Größenausschlusschromatographie mit gekoppelter Mehrwinkel-Laserlichtstreuung (GPC-MALLS) möglich waren. Durch dynamische Lichtstreuung (DLS) wurde das Löslichkeitsverhalten veranschaulicht. Sämtliche Produkte konnten zu Filmen verarbeitet werden, wobei Materialien mit DS 1,5-1,7 hohe Zugfestigkeiten (bis zu 42 MPa) und Elastizitätsmodule (bis 1390 MPa) aufwiesen. Insbesondere Stärkehexanoat mit DS <2 sowie Stärkebutanoat mit DS >2 hatten ein mechanisches Eigenschaftsprofil, welches insbesondere in Bezug auf die Festigkeit/Steifigkeit vergleichbar mit Verpackungsmaterialien wie Polyethylen war (Zugfestigkeit: 15-32 MPa, E-Modul: 300-1300 MPa). Zugfestigkeit und Elastizitätsmodul nahmen mit steigender Kettenlänge der veresterten Fettsäure ab. Ester längerkettiger Fettsäuren (C16-C18) waren spröde. Über Weitwinkel-Röntgenstreuung (WAXS) und Infrarotspektroskopie (ATR-FTIR) konnte der Verlauf der Festigkeiten mit einer zunehmenden Distanz der Stärke im Material begründet werden. Es konnten von DS und Kettenlänge abhängige Glasübergänge detektiert werden, die kristallinen Strukturen der langkettigen Fettsäuren zeigten einen Schmelzpeak. Die Hydrophobie der Filme wurde anhand von Kontaktwinkeln >95° gegen Wasser dargestellt. Blends mit biobasierten Polyterpenen sowie den in der Arbeit hergestellten Zein-Acylderivaten ermöglichten eine weitere Verbesserung der Zugfestigkeit bzw. des Elastizitätsmoduls hochsubstituierter Produkte. Eine thermoplastische Verarbeitung mittels Spritzgießen war sowohl für Produkte mit hohem als auch mittlerem DS-Wert ohne jeglichen Zusatz von Weichmachern möglich. Es entstanden homogene, transparente Prüfstäbe. Untersuchungen der Härte ergaben auch hier für Stärkehexanoat und –butanoat mit Polyethylen vergleichbare Werte. Ausgewählte Produkte wurden zu Fasern nach dem Schmelzspinnverfahren verarbeitet. Hierbei wurden insbesondere für hochsubstituierte Derivate homogenen Fasern erstellt, welche im Vergleich zur Gießfolie signifikant höhere Zugfestigkeiten aufwiesen. Stärkeester mit mittlerem DS ließen sich ebenfalls verarbeiten. Zunächst wurden für eine Übertragung des Konzeptes auf die Proteine Zein und WPI verschiedene Synthesemethoden verglichen. Die Veresterung mit Säurechloriden ergab hierbei die höchsten Werte. Im Hinblick auf eine gute Löslichkeit in organischen Lösungsmitteln wurde für WPI die Veresterung mit carbonyldiimidazol (CDI)-aktivierten Fettsäuren in DMSO und für Zein die Veresterung mit Säu-rechloriden in Pyridin bevorzugt. Es stellte sich heraus, dass acyliertes WPI zwar hydrophob, jedoch ohne Weichmacher nicht thermoplastisch verarbeitet werden konnte. Die Erstellung von Gießfolien führte zu Sprödbruchverhalten. Unter Zugabe der biobasierten Ölsäure wurde die Anwendung von acyliertem WPI als thermoplastischer Filler z. B. in Blends mit Stärkeestern dargestellt. Im Gegensatz hierzu zeigte acyliertes Zein Glasübergänge <100 °C bei ausreichender Stabilität (150-200 °C). Zeinoleat konnte ohne Weichmacher zu einer transparenten Gießfolie verarbeitet werden. Sämtliche Derivate erwiesen sich als ausgeprägt hydrophob. Zeinoleat konnte über das Schmelzspinnverfahren zu thermoplastischen Fasern verarbeitet werden.
The unicellular green alga Chlamydomonas reinhardtii is a long-established model organism for studies on photosynthesis and carbon metabolism-related physiology. Under conditions of air-level carbon dioxide concentration [CO2], a carbon concentrating mechanism (CCM) is induced to facilitate cellular carbon uptake. CCM increases the availability of carbon dioxide at the site of cellular carbon fixation. To improve our understanding of the transcriptional control of the CCM, we employed FAIRE-seq (formaldehyde-assisted Isolation of Regulatory Elements, followed by deep sequencing) to determine nucleosome-depleted chromatin regions of algal cells subjected to carbon deprivation. Our FAIRE data recapitulated the positions of known regulatory elements in the promoter of the periplasmic carbonic anhydrase (Cah1) gene, which is upregulated during CCM induction, and revealed new candidate regulatory elements at a genome-wide scale. In addition, time series expression patterns of 130 transcription factor (TF) and transcription regulator (TR) genes were obtained for cells cultured under photoautotrophic condition and subjected to a shift from high to low [CO2]. Groups of co-expressed genes were identified and a putative directed gene-regulatory network underlying the CCM was reconstructed from the gene expression data using the recently developed IOTA (inner composition alignment) method. Among the candidate regulatory genes, two members of the MYB-related TF family, Lcr1 (Low-CO2 response regulator 1) and Lcr2 (Low-CO2 response regulator 2), may play an important role in down-regulating the expression of a particular set of TF and TR genes in response to low [CO2]. The results obtained provide new insights into the transcriptional control of the CCM and revealed more than 60 new candidate regulatory genes. Deep sequencing of nucleosome-depleted genomic regions indicated the presence of new, previously unknown regulatory elements in the C. reinhardtii genome. Our work can serve as a basis for future functional studies of transcriptional regulator genes and genomic regulatory elements in Chlamydomonas.
Temperate forest soils of central Europe are regarded as important pools for soil organic carbon (SOC) and thought to have a high potential for carbon (C) sequestration. However, comprehensive data on total SOC storage, particularly under different forest types, and its drivers is limited. In this study, we analyzed a forest data set of 596 completely sampled soil profiles down to the parent material or to a depth of 1 m within Bavaria in southeast Germany in order to determine representative SOC stocks under different forest types in central Europe and the impact of different environmental parameters. We calculated a total median SOC stock of 9.8 kg m(-2) which is considerably lower compared with many other inventories within central Europe that used modelled instead of measured soil properties. Statistical analyses revealed climate as controlling parameter for the storage of SOC with increasing stocks in cool, humid mountainous regions and a strong decrease in areas with higher temperatures. No significant differences of total SOC storage were found between broadleaf, coniferous and mixed forests. However, coniferous forests stored around 35% of total SOC in the labile organic layer that is prone to human disturbance, forest fires and rising temperatures. In contrast, mixed and broadleaf forests stored the major part of SOC in the mineral soil. Moreover, these two forest types showed unchanged or even slightly increased mineral SOC stocks with higher temperatures, whereas SOC stocks in mineral soils under coniferous forest were distinctly lower. We conclude that mixed and broadleaf forests are more advantageous for C sequestration than coniferous forests. An intensified incorporation of broadleaf species in extent coniferous forests of Bavaria would prevent substantial SOC losses as a result of rising temperatures in the course of climate change.
Agricultural soils have a high potential for sequestration of atmospheric carbon due to their volume and several promising management options. However, there is a remarkable lack of information about the status quo of organic carbon in agricultural soils. In this study a comprehensive data set of 384 cropland soils and 333 grassland soils within the state of Bavaria in southeast Germany was analyzed in order to provide representative information on total amount, regional distribution and driving parameters of soil organic carbon (SOC) and nitrogen (N) in agricultural soils of central Europe. The results showed that grassland soils stored higher amounts of SOC (11.8 kg m(-2)) and N (0.92 kg m(-2)) than cropland soils (9.0 and 0.66 kg m(-2), respectively) due to moisture-induced accumulation of soil organic matter (SOM) in B horizons. Surprisingly, no distinct differences were found for the A horizons since tillage led to a relocation of SOM with depth in cropland soils. Statistical analyses of driving factors for SOM storage revealed soil moisture, represented by the topographic wetness index (TWI), as the most important parameter for both cropland and grassland soils. Climate effects (mean annual temperature and precipitation) were of minor importance in agricultural soils because management options counteracted them to a certain extent, particularly in cropland soils. The distribution of SOC and N stocks within Bavaria based on agricultural regions confirmed the importance of soil moisture since the highest cropland SOC and N stocks were found for tertiary hills and loess regions, which exhibited large areas with potentially high soil moisture content in extant floodplains. Grassland soils showed the highest accumulation of SOC and N in the Alps and Pre-Alps as a result of low temperatures, high amounts of precipitation and high soil moisture content in areas of glacial denudation. Soil class was identified as a further driving parameter for SOC and N storage in cropland soils. In total, cropland and grassland soils in Bavaria store 242 and 134 Mt SOC as well as 19 and 12 Mt N down to a soil depth of 1 m or the parent material, respectively.
Deep into the second half of the twentieth century the traditionalist definition of India as a country of villages remained dominant in official political rhetoric as well as cultural production. In the past two decades or so, this ruralist paradigm has been effectively superseded by a metropolitan imaginary in which the modern, globalised megacity increasingly functions as representative of India as a whole. Has the village, then, entirely vanished from the cultural imaginary in contemporary India? Addressing economic practices from upper-class consumerism to working-class family support strategies, this paper attempts to trace how ‘the village’ resurfaces or survives as a cultural reference point in the midst of the urban.
Deep into the second half of the twentieth century the traditionalist definition of India as a country of villages remained dominant in official political rhetoric as well as cultural production. In the past two decades or so, this ruralist paradigm has been effectively superseded by a metropolitan imaginary in which the modern, globalised megacity increasingly functions as representative of India as a whole. Has the village, then, entirely vanished from the cultural imaginary in contemporary India? Addressing economic practices from upper-class consumerism to working-class family support strategies, this paper attempts to trace how 'the village' resurfaces or survives as a cultural reference point in the midst of the urban.
Gleichheit
(2013)