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  • 1
    Electronic Resource
    Electronic Resource
    Springer
    Topics in catalysis 8 (1999), S. 211-222 
    ISSN: 1572-9028
    Keywords: reforming ; methane ; carbon dioxide ; Rh/SiO2 ; vanadia-promoted Rh/SiO2 ; FTIR spectroscopy
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The reforming of methane with carbon dioxide over rhodium dispersed on silica, Rh/SiO2, and vanadia-promoted silica, Rh/VOx/SiO2, was studied by kinetic test reactions under differential conditions in a temperature range from 723 to 773 K. Transmission infrared spectroscopy was applied to observe the interaction of CO2 with the catalysts and the formation of surface intermediates during the CO2–CH4 reforming reaction. To analyze carbon deposition XP spectroscopy and TPO was carried out. It has been shown that the promotion of Rh/SiO2 catalysts with vanadium oxide enhances the catalytic activity for CO2 reforming of methane and decreases the deactivation by carbon deposition. This is attributed to the formation of a partial VOx overlayer on the Rh surface, which reduces the size of accessible ensembles of Rh atoms required for coke formation and creates new sites at the Rh–VOx interfacial region that are considered to be active sites for the activation/dissociation of carbon dioxide.
    Type of Medium: Electronic Resource
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  • 2
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    Copernicus Publications (EGU)
    In:  Earth System Science Data, 9 . pp. 809-831.
    Publication Date: 2020-02-06
    Description: The injection of sulphur into the stratosphere by explosive volcanic eruptions is the cause of significant climate variability. Based on sulphate records from a suite of ice cores from Greenland and Antarctica, the eVolv2k database includes estimates of the magnitudes and approximate source latitudes of major volcanic stratospheric sulphur injection (VSSI) events from 500 BCE to 1900 CE, constituting an update of prior reconstructions and an extension of the record by 1000 years. The VSSI estimates incorporate improvements to the ice core records in terms of synchronization and dating, refinements to the methods used to estimate VSSI from ice core records, and includes first estimates of the random uncertainties in VSSI values. VSSI estimates for many of the largest eruptions, including Samalas (1257), Tambora (1815) and Laki (1783) are within 10% of prior estimates. A number of strong events are included in eVolv2k which are largely underestimated or not included in earlier VSSI reconstructions, including events in 540, 574, 682 and 1108 CE. The long term annual mean VSSI from major volcanic eruptions is estimated to be ∼ 0.5 Tg [S] yr−1, ∼ 50 % greater than a prior reconstruction, due to the identification of more events and an increase in the magnitude of many intermediate events. A long-term, latitudinally and monthly resolved stratospheric aerosol optical depth (SAOD) time series is reconstructed from the eVolv2k VSSI estimates, and the resulting global mean SAOD is found to be similar (within 33%) to a prior reconstruction for most of the largest eruptions. The long-term (500 BCE–900 CE) average global mean SAOD estimated from the eVolv2k VSSI estimates and including a constant "background" injection of stratospheric sulphur is ∼ 0.014, 30 % greater than a prior reconstruction. These new long-term reconstructions of past VSSI and SAOD variability give context to recent volcanic forcing, suggesting that the 20th century was a period of somewhat weaker than average volcanic forcing, with current best estimates of 20th century mean VSSI and SAOD values being 25 and 14 % less, respectively, than the mean of the 500 BCE to 1900 CE period. The reconstructed VSSI and SAOD data are available at https://doi.org/10.1594/WDCC/eVolv2k_v2〉.
    Type: Article , PeerReviewed
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  • 3
    Publication Date: 2020-02-06
    Description: The pre-industrial millennium is among the periods selected by the Paleoclimate Model Intercomparison Project (PMIP) for experiments contributing to the sixth phase of the Coupled Model Intercomparison Project (CMIP6) and the fourth phase of the PMIP (PMIP4). The past1000 transient simulations serve to investigate the response to (mainly) natural forcing under background conditions not too different from today, and to discriminate between forced and internally generated variability on interannual to centennial timescales. This paper describes the motivation and the experimental set-ups for the PMIP4-CMIP6 past1000 simulations, and discusses the forcing agents orbital, solar, volcanic, and land use/land cover changes, and variations in greenhouse gas concentrations. The past1000 simulations covering the pre-industrial millennium from 850 Common Era (CE) to 1849 CE have to be complemented by historical simulations (1850 to 2014 CE) following the CMIP6 protocol. The external forcings for the past1000 experiments have been adapted to provide a seamless transition across these time periods. Protocols for the past1000 simulations have been divided into three tiers. A default forcing data set has been defined for the Tier 1 (the CMIP6 past1000) experiment. However, the PMIP community has maintained the flexibility to conduct coordinated sensitivity experiments to explore uncertainty in forcing reconstructions as well as parameter uncertainty in dedicated Tier 2 simulations. Additional experiments (Tier 3) are defined to foster collaborative model experiments focusing on the early instrumental period and to extend the temporal range and the scope of the simulations. This paper outlines current and future research foci and common analyses for collaborative work between the PMIP and the observational communities (reconstructions, instrumental data).
    Type: Article , PeerReviewed
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    Format: archive
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  • 4
    Publication Date: 2020-02-06
    Description: Significance: Cold and dry glacial-state climate conditions persisted in the Southern Hemisphere until approximately 17.7 ka, when paleoclimate records show a largely unexplained sharp, nearly synchronous acceleration in deglaciation. Detailed measurements in Antarctic ice cores document exactly at that time a unique, ∼192-y series of massive halogen-rich volcanic eruptions geochemically attributed to Mount Takahe in West Antarctica. Rather than a coincidence, we postulate that halogen-catalyzed stratospheric ozone depletion over Antarctica triggered large-scale atmospheric circulation and hydroclimate changes similar to the modern Antarctic ozone hole, explaining the synchronicity and abruptness of accelerated Southern Hemisphere deglaciation. Abstract: Glacial-state greenhouse gas concentrations and Southern Hemisphere climate conditions persisted until ∼17.7 ka, when a nearly synchronous acceleration in deglaciation was recorded in paleoclimate proxies in large parts of the Southern Hemisphere, with many changes ascribed to a sudden poleward shift in the Southern Hemisphere westerlies and subsequent climate impacts. We used high-resolution chemical measurements in the West Antarctic Ice Sheet Divide, Byrd, and other ice cores to document a unique, ∼192-y series of halogen-rich volcanic eruptions exactly at the start of accelerated deglaciation, with tephra identifying the nearby Mount Takahe volcano as the source. Extensive fallout from these massive eruptions has been found 〉2,800 km from Mount Takahe. Sulfur isotope anomalies and marked decreases in ice core bromine consistent with increased surface UV radiation indicate that the eruptions led to stratospheric ozone depletion. Rather than a highly improbable coincidence, circulation and climate changes extending from the Antarctic Peninsula to the subtropics—similar to those associated with modern stratospheric ozone depletion over Antarctica—plausibly link the Mount Takahe eruptions to the onset of accelerated Southern Hemisphere deglaciation ∼17.7 ka.
    Type: Article , PeerReviewed
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  • 5
    Publication Date: 2021-02-08
    Description: The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 "year without a summer", and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic sulfate signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), five state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora) and volcanic (with Tambora) sulfate deposition to polar regions and compare to ice core records. The models simulate overall similar patterns of background sulfate deposition, al-though there are differences in regional details and magnitude. However, the volcanic sulfate deposition varies considerably between the models with differences in timing, spatial pattern and magnitude. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kgkm-2 and on Greenland from 31 to 194 kgkm-2, as compared to the mean ice-corederived estimates of roughly 50 kgkm-2 for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results suggest that deriving relationships between sulfate deposited on ice sheets and atmospheric sulfate burdens from model simulations may be associated with greater uncertainties than previously thought.
    Type: Article , PeerReviewed , info:eu-repo/semantics/article
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  • 6
    Publication Date: 2019-09-23
    Description: Assessments of climate sensitivity to projected greenhouse gas concentrations underpin environmental policy decisions, with such assessments often based on model simulations of climate during recent centuries and millennia1, 2, 3. These simulations depend critically on accurate records of past aerosol forcing from global-scale volcanic eruptions, reconstructed from measurements of sulphate deposition in ice cores4, 5, 6. Non-uniform transport and deposition of volcanic fallout mean that multiple records from a wide array of ice cores must be combined to create accurate reconstructions. Here we re-evaluated the record of volcanic sulphate deposition using a much more extensive array of Antarctic ice cores. In our new reconstruction, many additional records have been added and dating of previously published records corrected through precise synchronization to the annually dated West Antarctic Ice Sheet Divide ice core7, improving and extending the record throughout the Common Era. Whereas agreement with existing reconstructions is excellent after 1500, we found a substantially different history of volcanic aerosol deposition before 1500; for example, global aerosol forcing values from some of the largest eruptions (for example, 1257 and 1458) previously were overestimated by 20–30% and others underestimated by 20–50%.
    Type: Article , PeerReviewed
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  • 7
    Publication Date: 2019-02-01
    Description: Volcanic activity in and around the year 536 CE led to severe cold and famine, and has been speculatively linked to large-scale societal crises around the globe. Using a coupled aerosol-climate model, with eruption parameters constrained by recently re-dated ice core records and historical observations of the aerosol cloud, we reconstruct the radiative forcing resulting from a sequence of two major volcanic eruptions in 536 and 540 CE. We estimate that the decadal-scale Northern Hemisphere (NH) extra-tropical radiative forcing from this volcanic “double event” was larger than that of any period in existing reconstructions of the last 1200 years. Earth system model simulations including the volcanic forcing show peak NH mean temperature anomalies reaching more than −2 °C, and show agreement with the limited number of available maximum latewood density temperature reconstructions. The simulations also produce decadal-scale anomalies of Arctic sea ice. The simulated cooling is interpreted in terms of probable impacts on agricultural production in Europe, and implies a high likelihood of multiple years of significant decreases in crop production across Scandinavia, supporting the theory of a connection between the 536 and 540 eruptions and evidence of societal crisis dated to the mid-6th century.
    Type: Article , PeerReviewed
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  • 8
    Publication Date: 2022-01-31
    Description: Extratropical volcanic eruptions are commonly thought to be less effective at driving large-scale surface cooling than tropical eruptions. However, recent minor extratropical eruptions have produced a measurable climate impact, and proxy records suggest that the most extreme Northern Hemisphere cold period of the Common Era was initiated by an extratropical eruption in 536 CE. Using ice-core-derived volcanic stratospheric sulfur injections and Northern Hemisphere summer temperature reconstructions from tree rings, we show here that in proportion to their estimated stratospheric sulfur injection, extratropical explosive eruptions since 750 CE have produced stronger hemispheric cooling than tropical eruptions. Stratospheric aerosol simulations demonstrate that for eruptions with a sulfur injection magnitude and height equal to that of the 1991 Mount Pinatubo eruption, extratropical eruptions produce time-integrated radiative forcing anomalies over the Northern Hemisphere extratropics up to 80% greater than tropical eruptions, as decreases in aerosol lifetime are overwhelmed by the enhanced radiative impact associated with the relative confinement of aerosol to a single hemisphere. The model results are consistent with the temperature reconstructions, and elucidate how the radiative forcing produced by extratropical eruptions is strongly dependent on the eruption season and sulfur injection height within the stratosphere.
    Type: Article , PeerReviewed
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  • 9
    Publication Date: 2024-02-07
    Description: We present a transient simulation of global vegetation and climate patterns of the mid- and late Holocene using the MPI-ESM (Max Planck Institute for Meteorology Earth System Model) at T63 resolution. The simulated vegetation trend is discussed in the context of the simulated Holocene climate change. Our model captures the main trends found in reconstructions. Most prominent are the southward retreat of the northern treeline that is combined with the strong decrease of forest in the high northern latitudes during the Holocene and the vast increase of the Saharan desert, embedded in a general decrease in precipitation and vegetation in the Northern Hemisphere monsoon margin regions. The Southern Hemisphere experiences weaker changes in total vegetation cover during the last 8000 years. However, the monsoon-related increase in precipitation and the insolation-induced cooling of the winter climate lead to shifts in the vegetation composition, mainly between the woody plant functional types (PFTs). The large-scale global patterns of vegetation almost linearly follow the subtle, approximately linear, orbital forcing. In some regions, however, non-linear, more rapid changes in vegetation are found in the simulation. The most striking region is the Sahel–Sahara domain with rapid vegetation transitions to a rather desertic state, despite a gradual insolation forcing. Rapid shifts in the simulated vegetation also occur in the high northern latitudes, in South Asia and in the monsoon margins of the Southern Hemisphere. These rapid changes are mainly triggered by changes in the winter temperatures, which go into, or move out of, the bioclimatic tolerance range of individual PFTs. The dynamics of the transitions are determined by dynamics of the net primary production (NPP) and the competition between PFTs. These changes mainly occur on timescales of centuries. More rapid changes in PFTs that occur within a few decades are mainly associated with the timescales of mortality and the bioclimatic thresholds implicit in the dynamic vegetation model, which have to be interpreted with caution. Most of the simulated Holocene vegetation changes outside the high northern latitudes are associated with modifications in the intensity of the global summer monsoon dynamics that also affect the circulation in the extra tropics via teleconnections. Based on our simulations, we thus identify the global monsoons as the key player in Holocene climate and vegetation change.
    Type: Article , PeerReviewed
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  • 10
    Publication Date: 2023-01-13
    Keywords: Age; AGE; Ammonium; Bismuth; Black carbon; Calcium; Colle_Gnifetti_composite; Colle Gnifetti, Monte Rosa, Swiss Alps; COMPCORE; Composite Core; ICP-Q-MS; Inductively coupled plasma-quadrupole-mass spectrometry; Ion chromatography; Lead; Nitrate; Sodium; SP2 soot photometry; Sulfate
    Type: Dataset
    Format: text/tab-separated-values, 2977 data points
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