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  • Copernicus  (23)
  • American Association for the Advancement of Science
  • American Association for the Advancement of Science (AAAS)
  • 2010-2014  (28)
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  • 1
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    Palladium-catalyzed aerobic dehydrogenation of substituted cyclohexanones to phenols (2011)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2011-06-11
    Description: Aromatic molecules are key constituents of many pharmaceuticals, electronic materials, and commodity plastics. The utility of these molecules directly reflects the identity and pattern of substituents on the aromatic ring. Here, we report a palladium(II) catalyst system, incorporating an unconventional ortho-dimethylaminopyridine ligand, for the conversion of substituted cyclohexanones to the corresponding phenols. The reaction proceeds via successive dehydrogenation of two saturated carbon-carbon bonds of the six-membered ring and uses molecular oxygen as the hydrogen acceptor. This reactivity demonstrates a versatile and efficient strategy for the synthesis of substituted aromatic molecules with fundamentally different selectivity constraints from the numerous known synthetic methods that rely on substitution of a preexisting aromatic ring.〈br /〉〈br /〉〈a href="https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3174491/" target="_blank"〉〈img src="https://static.pubmed.gov/portal/portal3rc.fcgi/4089621/img/3977009" border="0"〉〈/a〉   〈a href="https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3174491/" target="_blank"〉This paper as free author manuscript - peer-reviewed and accepted for publication〈/a〉〈br /〉〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Izawa, Yusuke -- Pun, Doris -- Stahl, Shannon S -- RC1 GM091161/GM/NIGMS NIH HHS/ -- RC1 GM091161-01/GM/NIGMS NIH HHS/ -- RC1 GM091161-02/GM/NIGMS NIH HHS/ -- RC1-GM091161/GM/NIGMS NIH HHS/ -- New York, N.Y. -- Science. 2011 Jul 8;333(6039):209-13. doi: 10.1126/science.1204183. Epub 2011 Jun 9.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Department of Chemistry, University of Wisconsin-Madison, Madison, WI 53706, USA.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/21659567" target="_blank"〉PubMed〈/a〉
    Keywords: Aerobiosis ; Catalysis ; Cyclohexanones/*chemistry ; Hydrogen/chemistry ; Kinetics ; Ligands ; Molecular Structure ; Organic Chemistry Processes ; Palladium/*chemistry ; Phenols/*chemical synthesis/*chemistry
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
    Published by American Association for the Advancement of Science (AAAS)
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  • 2
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    Synthesis of methylphosphonic acid by marine microbes: a source for methane in the aerobic ocean (2012)
    American Association for the Advancement of Science (AAAS)
    Details
    Publication Date: 2012-09-01
    Description: Relative to the atmosphere, much of the aerobic ocean is supersaturated with methane; however, the source of this important greenhouse gas remains enigmatic. Catabolism of methylphosphonic acid by phosphorus-starved marine microbes, with concomitant release of methane, has been suggested to explain this phenomenon, yet methylphosphonate is not a known natural product, nor has it been detected in natural systems. Further, its synthesis from known natural products would require unknown biochemistry. Here we show that the marine archaeon Nitrosopumilus maritimus encodes a pathway for methylphosphonate biosynthesis and that it produces cell-associated methylphosphonate esters. The abundance of a key gene in this pathway in metagenomic data sets suggests that methylphosphonate biosynthesis is relatively common in marine microbes, providing a plausible explanation for the methane paradox.〈br /〉〈br /〉〈a href="https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3466329/" target="_blank"〉〈img src="https://static.pubmed.gov/portal/portal3rc.fcgi/4089621/img/3977009" border="0"〉〈/a〉   〈a href="https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3466329/" target="_blank"〉This paper as free author manuscript - peer-reviewed and accepted for publication〈/a〉〈br /〉〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Metcalf, William W -- Griffin, Benjamin M -- Cicchillo, Robert M -- Gao, Jiangtao -- Janga, Sarath Chandra -- Cooke, Heather A -- Circello, Benjamin T -- Evans, Bradley S -- Martens-Habbena, Willm -- Stahl, David A -- van der Donk, Wilfred A -- F32 GM095024/GM/NIGMS NIH HHS/ -- P001 GM077596/GM/NIGMS NIH HHS/ -- P01 GM077596/GM/NIGMS NIH HHS/ -- S10 RR028833/RR/NCRR NIH HHS/ -- Howard Hughes Medical Institute/ -- New York, N.Y. -- Science. 2012 Aug 31;337(6098):1104-7. doi: 10.1126/science.1219875.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉Institute for Genomic Biology, University of Illinois, Urbana, IL 61801, USA. metcalf@uiuc.edu〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/22936780" target="_blank"〉PubMed〈/a〉
    Keywords: Aerobiosis ; Aquatic Organisms/genetics/*metabolism ; Archaea/genetics/*metabolism ; Archaeal Proteins/classification/genetics/*metabolism ; Dioxygenases/classification/genetics/metabolism ; Gene Order ; Metagenome ; Methane/*biosynthesis ; Organophosphorus Compounds/*metabolism ; Phylogeny ; Seawater/chemistry/microbiology
    Print ISSN: 0036-8075
    Electronic ISSN: 1095-9203
    Topics: Biology , Chemistry and Pharmacology , Computer Science , Medicine , Natural Sciences in General , Physics
    Published by American Association for the Advancement of Science (AAAS)
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  • 3
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    Asynchronism in leaf and wood production in tropical forests: a study combining satellite and ground-based measurements (2013)
    Copernicus
    Details
    Publication Date: 2013-05-16
    Description: The fixation of carbon in tropical forests mainly occurs through the production of wood and leaves, both being the principal components of net primary production. Currently field and satellite observations are independently used to describe the forest carbon cycle, but the link between satellite-derived forest phenology and field-derived forest productivity remains opaque. We used a unique combination of a MODIS EVI dataset, a climate-explicit wood production model and direct litterfall observations at an intra-annual time scale in order to question the synchronism of leaf and wood production in tropical forests. Even though leaf and wood biomass fluxes had the same range (respectively 2.4 ± 1.4 Mg C ha−1yr−1 and 2.2 ± 0.4 Mg C ha−1yr−1), they occured separately in time. EVI increased with the magnitude of leaf renewal at the beginning of the dry season when solar irradiance was at its maximum. At this time, wood production stopped. At the onset of the rainy season when new leaves were fully mature and water available again, wood production quickly increased to reach its maximum in less than a month, reflecting a change in carbon allocation from short lived pools (leaves) to long lived pools (wood). The time lag between peaks of EVI and wood production (109 days) revealed a substantial decoupling between the irradiance-driven leaf renewal and the water-driven wood production. Our work is a first attempt to link EVI data, wood production and leaf phenology at a seasonal time scale in a tropical evergreen rainforest and pave the way to develop more sophisticated global carbon cycle models in tropical forests.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
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    Exploring the link between drought indicators and impacts (2014)
    Copernicus
    Details
    Publication Date: 2014-12-15
    Description: Current drought monitoring and early warning systems use different indicators for monitoring drought conditions and apply different indicator thresholds and rules for assigning drought intensity classes or issue warnings or alerts. Nevertheless, there is little knowledge on the meaning of different hydro-meteorologic indicators for impact occurrence on the ground. To date, there have been very few attempts to systematically characterize the indicator–impact-relationship owing to the sparse and patchy data for ground truthing hydro-meteorologic variables. The newly established European Drought Impact report Inventory (EDII) offers the possibility to investigate this linkage. The aim of this study was to explore the link between hydro-meteorologic indicators and drought impacts for the case study area Germany and thus to test the potential of qualitative impact data for evaluating the performance of drought indicators. As drought indicators two climatological drought indices as well as streamflow and groundwater level percentiles were selected. Linkage was assessed though data visualization and correlation analysis between monthly timeseries of indicator–impact data at the federal state level, and between spatial patterns for selected drought events. The analysis clearly revealed a significant moderate to strong correlation for some states and drought events allowing for an intercomparison of the performance of different drought indicators. While several commonalities could be identified regarding "best" indicator, indicator metric, and time-scale of climatic anomaly, the analysis also exposed differences among federal states and drought events, suggesting that the linkage is time-variant and region specific to some degree. Concerning thresholds associated with drought impact onset, we found that no single "best" threshold value can be identified but impacts occur within a range of indicator values. While the findings strongly depend on data and may change with a growing number of EDII entries in the future, this study clearly demonstrates the feasibility of ground truthing hydro-meteorologic variables with text-based impact reports and highlights the value of impact reporting as a tool for monitoring drought conditions.
    Electronic ISSN: 2195-9269
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
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    Streamflow trends in Europe: evidence from a dataset of near-natural catchments (2010)
    Copernicus
    Details
    Publication Date: 2010-12-01
    Description: Streamflow observations from near-natural catchments are of paramount importance for detection and attribution studies, evaluation of large-scale model simulations, and assessment of water management, adaptation and policy options. This study investigates streamflow trends in a newly-assembled, consolidated dataset of near-natural streamflow records from 441 small catchments in 15 countries across Europe. The period 1962–2004 provided the best spatial coverage, but analyses were also carried out for longer time periods (with fewer stations), starting in 1932, 1942 and 1952. Trends were calculated by the slopes of the Kendall-Theil robust line for standardized annual and monthly streamflow, as well as for summer low flow magnitude and timing. A regionally coherent picture of annual streamflow trends emerged, with negative trends in southern and eastern regions, and generally positive trends elsewhere. Trends in monthly streamflow for 1962–2004 elucidated potential causes for these changes, as well as for changes in hydrological regimes across Europe. Positive trends were found in the winter months in most catchments. A marked shift towards negative trends was observed in April, gradually spreading across Europe to reach a maximum extent in August. Low flows have decreased in most regions where the lowest mean monthly flow occurs in summer, but vary for catchments which have flow minima in winter and secondary low flows in summer. The study largely confirms findings from national and regional scale trend analyses, but clearly adds to these by confirming that these tendencies are part of coherent patterns of change, which cover a much larger region. The broad, continental-scale patterns of change are mostly congruent with the hydrological responses expected from future climatic changes, as projected by climate models. The patterns observed could hence provide a valuable benchmark for a number of different studies and model simulations.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
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    Low-frequency variability of European runoff (2011)
    Copernicus
    Details
    Publication Date: 2011-09-13
    Description: This study investigates the low-frequency components of observed monthly river flow from a large number of small catchments in Europe. The low-frequency components, defined as fluctuations on time scales longer than one year, were analysed both with respect to their dominant space-time patterns as well as their contribution to the variance of monthly runoff. The analysis of observed streamflow and corresponding time series of precipitation and temperature, showed that the fraction of low-frequency variance of runoff is on average larger than, and not correlated to, the fraction of low-frequency variance of precipitation and temperature. However, it is correlated with mean climatic conditions and is on average lowest in catchments with significant influence of snow. Furthermore, it increases (decreases) under drier (wetter) conditions – indicating that the average degree of catchment wetness may be a primary control of low-frequency runoff dynamics. The fraction of low-frequency variance of runoff is consistently lower in responsive catchments, with a high variability of daily runoff. The dominant space-time patterns of low-frequency runoff in Europe, identified using nonlinear dimension reduction, revealed that low-frequency runoff can be described with three modes, explaining together 80.6% of the variance. The dominant mode has opposing centres of simultaneous variations in northern and southern Europe. The secondary mode features a west-east pattern and the third mode has its centre of influence in central Europe. All modes are closely related to the space-time patterns extracted from time series of precipitation and temperature. In summary, it is shown that the dynamics of low-frequency runoff follows well known continental-scale atmospheric features, whereas the proportion of variance attributed to low-frequency fluctuations is controlled by catchment processes and varies with mean climatic conditions. The results may have implications for interpreting the impact of changes in temperature and precipitation on river-flow dynamics.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
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    The influence of decadal-scale variability on trends in long European streamflow records (2013)
    Copernicus
    Details
    Publication Date: 2013-07-15
    Description: This study seeks to provide a long-term context for the growing number of trend analyses which have been applied to river flows in Europe. Most studies apply trend tests to fixed periods, in relatively short (generally 1960s–present) records. This study adopts an alternative "multi-temporal" approach, whereby trends are fitted to every possible combination of start and end years in a record. The method is applied to 132 catchments with long (1932–2004) hydrometric records from northern and central Europe, which were chosen as they are minimally anthropogenically influenced and have good quality data. The catchments are first clustered into five regions, which are broadly homogenous in terms of interdecadal variability of annual mean flow. The multi-temporal trend approach was then applied to regional time series of different hydrological indicators (annual, monthly and high and low flows). The results reveal that the magnitude and even direction of short-term trends are heavily influenced by interdecadal variability. Some short-term trends revealed in previous studies are shown to be unrepresentative of long-term change. For example, previous studies have identified post-1960 river flow decreases in southern and eastern Europe: in parts of eastern Europe, these trends are resilient to study period, extending back to the 1930s; in southern France, longer records show evidence of positive trends which reverse from the 1960s. Recent (post-1960) positive trends in northern Europe are also not present in longer records, due to decadal variations influenced by the North Atlantic Oscillation. The results provide a long-term reference for comparison with published and future studies. The multi-temporal approach advocated here is recommended for use in future trend assessments, to help contextualise short-term trends. Future work should also attempt to explain the decadal-scale variations that drive short-term trends, and thus develop more sophisticated methods for trend detection that take account of interdecadal variability and its drivers.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
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    Are streamflow recession characteristics really characteristic? (2013)
    Copernicus
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    Publication Date: 2013-02-27
    Description: Streamflow recession has been investigated by a variety of methods, often involving the fit of a model to empirical recession plots to parameterize a non-linear storage–outflow relationship based on the dQ/dt−Q method. Such recession analysis methods (RAMs) are used to estimate hydraulic conductivity, storage capacity, or aquifer thickness and to model streamflow recession curves for regionalization and prediction at the catchment scale. Numerous RAMs have been published, but little is known about how comparably the resulting recession models distinguish characteristic catchment behavior. In this study we combined three established recession extraction methods with three different parameter-fitting methods to the power-law storage–outflow model to compare the range of recession characteristics that result from the application of these different RAMs. Resulting recession characteristics including recession time and corresponding storage depletion were evaluated for 20 meso-scale catchments in Germany. We found plausible ranges for model parameterization; however, calculated recession characteristics varied over two orders of magnitude. While recession characteristics of the 20 catchments derived with the different methods correlate strongly, particularly for the RAMs that use the same extraction method, not all rank the catchments consistently, and the differences among some of the methods are larger than among the catchments. To elucidate this variability we discuss the ambiguous roles of recession extraction procedures and the parameterization of the storage–outflow model and the limitations of the presented recession plots. The results suggest strong limitations to the comparability of recession characteristics derived with different methods, not only in the model parameters but also in the relative characterization of different catchments. A multiple-methods approach to investigating streamflow recession characteristics should be considered for applications whenever possible.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
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  • 9
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    Sensitivity of a data-driven soil water balance model to estimate summer evapotranspiration along a forest chronosequence (2011)
    Copernicus
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    Publication Date: 2011-11-17
    Description: The hydrology of ecosystem succession gives rise to new challenges for the analysis and modelling of water balance components. Recent large-scale alterations of forest cover across the globe suggest that a significant portion of new biophysical environments will influence the long-term dynamics and limits of water fluxes compared to pre-succession conditions. This study assesses the estimation of summer evapotranspiration along three FLUXNET sites at Campbell River, British Columbia, Canada using a data-driven soil water balance model validated by Eddy Covariance measurements. It explores the sensitivity of the model to different forest succession states, a wide range of computational time steps, rooting depths, and canopy interception capacity values. Uncertainty in the measured EC fluxes resulting in an energy imbalance was consistent with previous studies and does not affect the validation of the model. The agreement between observations and model estimates proves that the usefulness of the method to predict summer AET over mid- and long-term periods is independent of stand age. However, an optimal combination of the parameters rooting depth, time step and interception capacity threshold is needed to avoid an underestimation of AET as seen in past studies. The study suggests that summer AET could be estimated and monitored in many more places than those equipped with Eddy Covariance or sap-flow measurements to advance the understanding of water balance changes in different successional ecosystems.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
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  • 10
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    Comparison of hydrological model structures based on recession and low flow simulations (2011)
    Copernicus
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    Publication Date: 2011-11-17
    Description: Low flows are often poorly reproduced by commonly used hydrological models, which are traditionally designed to meet peak flow situations. Hence, there is a need to improve hydrological models for low flow prediction. This study assessed the impact of model structure on low flow simulations and recession behaviour using the Framework for Understanding Structural Errors (FUSE). FUSE identifies the set of subjective decisions made when building a hydrological model and provides multiple options for each modeling decision. Altogether 79 models were created and applied to simulate stream flows in the snow dominated headwater catchment Narsjø in Norway (119 km2). All models were calibrated using an automatic optimisation method. The results showed that simulations of summer low flows were poorer than simulations of winter low flows, reflecting the importance of different hydrological processes. The model structure influencing winter low flow simulations is the lower layer architecture, whereas various model structures were identified to influence model performance during summer.
    Print ISSN: 1027-5606
    Electronic ISSN: 1607-7938
    Topics: Geography , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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