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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
    Publication Date: 2019-07-17
    Description: Volcanism is a natural climate forcing causing short-term variations in temperatures. Histories of volcanic eruptions are needed to quantify their role in climate variability and assess human impacts. We present two new seasonally resolved, annually dated non-sea-salt sulfur records from polar ice cores - WAIS Divide (WDC06A) from West Antarctica spanning 408 B.C.E. to 2003 C.E. and NEEM (NEEM-2011-S1) from Greenland spanning 78 to 1997 C.E. - both analyzed using high-resolution continuous flow analysis coupled to two mass spectrometers. The high dating accuracy allowed placing the large bi-hemispheric deposition event ascribed to the eruption of Kuwae in Vanuatu (previously thought to be 1452/1453 C.E. and used as a tie-point in ice core dating) into the year 1458/1459 C.E. This new age is consistent with an independent ice core timescale from Law Dome and explains an apparent delayed response in tree rings to this volcanic event. A second volcanic event is detected in 1453 C.E. in both ice cores. We show for the first time ice core signals in Greenland and Antarctica from the strong eruption of Taupo in New Zealand in 232 C.E. In total, 133 volcanic events were extracted from WDC06A and 138 from NEEM-2011-S1, with 50 ice core signals - predominantly from tropical source volcanoes - identified simultaneously in both records. We assess the effect of large bipolar events on temperature-sensitive tree ring proxies. These two new volcanic records, synchronized with available ice core records to account for spatial variability in sulfate deposition, provide a basis for improving existing time series of volcanic forcing.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 3
    Publication Date: 2020-07-28
    Description: The assassination of Julius Caesar in 44 BCE triggered a power struggle that ultimately ended the Roman Republic and, eventually, the Ptolemaic Kingdom, leading to the rise of the Roman Empire. Climate proxies and written documents indicate that this struggle occurred during a period of unusually inclement weather, famine, and disease in the Mediterranean region; historians have previously speculated that a large volcanic eruption of unknown origin was the most likely cause. Here we show using well-dated volcanic fallout records in six Arctic ice cores that one of the largest volcanic eruptions of the past 2,500 y occurred in early 43 BCE, with distinct geochemistry of tephra deposited during the event identifying the Okmok volcano in Alaska as the source. Climate proxy records show that 43 and 42 BCE were among the coldest years of recent millennia in the Northern Hemisphere at the start of one of the coldest decades. Earth system modeling suggests that radiative forcing from this massive, high-latitude eruption led to pronounced changes in hydroclimate, including seasonal temperatures in specific Mediterranean regions as much as 7 °C below normal during the 2 y period following the eruption and unusually wet conditions. While it is difficult to establish direct causal linkages to thinly documented historical events, the wet and very cold conditions from this massive eruption on the opposite side of Earth probably resulted in crop failures, famine, and disease, exacerbating social unrest and contributing to political realignments throughout the Mediterranean region at this critical juncture of Western civilization.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 4
    Publication Date: 2016-11-14
    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%.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 5
    Publication Date: 2017-01-24
    Description: Advances in trace gas analysis allow localised, non-atmospheric features to be resolved in ice cores, superimposed on the coherent atmospheric signal. These highfrequency signals could not have survived the low-pass filter effect that gas diffusion in the firn exerts on the atmospheric history and therefore do not result from changes in the atmospheric composition at the ice sheet surface. Using continuous methane (CH4) records obtained from five polar ice cores, we characterise these non-atmospheric signals and explore their origin. Isolated samples, enriched in CH4 in the Tunu13 (Greenland) record are linked to the presence of melt layers. Melting can enrich the methane concentration due to a solubility effect, but we find that an additional in situ process is required to generate the full magnitude of these anomalies. Furthermore, in all the ice cores studied there is evidence of reproducible, decimetre-scale CH4 variability. Through a series of tests, we demonstrate that this is an artifact of layered bubble trapping in a heterogeneousdensity firn column; we use the term “trapping signal” for this phenomenon. The peak-to-peak amplitude of the trapping signal is typically 5 ppb, but may exceed 40 ppb. Signal magnitude increases with atmospheric CH4 growth rate and seasonal density contrast, and decreases with accumulation rate. Significant annual periodicity is present in the CH4 variability of two Greenland ice cores, suggesting that layered gas trapping at these sites is controlled by regular, seasonal variations in the physical properties of the firn. Future analytical campaigns should anticipate high-frequency artifacts at high-melt ice core sites or during time periods with high atmospheric CH4 growth rate in order to avoid misinterpretation of such features as past changes in atmospheric composition.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 6
    Publication Date: 2018-01-02
    Description: 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.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 7
    Publication Date: 2015-12-17
    Description: Continental dust plays an important role in climate forcing, by interacting with incoming solar and outgoing long wave radiation and by impacting albedo when deposited on bright surfaces such as fresh snow. Continental dust may also play an important role in ocean fertilization and carbon sequestration. Because the lifetime of dust aerosol in the atmosphere is only on the order of days to weeks, spatial and temporal variability in concentrations and fluxes is high and understanding of recent and long term changes is limited. Therefore, understanding of natural variations and climate drivers of continental dust, and potential climate feedbacks on longer timescales is critical. Here we present and discuss continuous, high depth resolution measurements of a range of dust proxies in high latitude ice cores from the Arctic and Antarctic. Sub-annually resolved measurements provide insights into the temporal variations in dust deposition. Included are traditional proxies such as non-sea-salt (nss) calcium and insoluble particle number and size distribution as well as less traditional proxies such as rare earth elements which together provide important insights into how dust sources and transport may have changed in the past. We compare these detailed dust records with climate and land use proxies to investigate drivers of dustiness during the last three millennium.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Conference , notRev
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  • 8
    Publication Date: 2019-07-17
    Description: Past global climate changes had strong regional expression. To elucidate their spatio-temporal pattern, we reconstructed past temperatures for seven continental-scale regions during the past one to two millennia. The most coherent feature in nearly all of the regional temperature reconstructions is a long-term cooling trend, which ended late in the nineteenth century. At multi-decadal to centennial scales, temperature variability shows distinctly different regional patterns, with more similarity within each hemisphere than between them. There were no globally synchronous multi-decadal warm or cold intervals that define a worldwide Medieval Warm Period or Little Ice Age, but all reconstructions show generally cold conditions between ad 1580 and 1880, punctuated in some regions by warm decades during the eighteenth century. The transition to these colder conditions occurred earlier in the Arctic, Europe and Asia than in North America or the Southern Hemisphere regions. Recent warming reversed the long-term cooling; during the period ad 1971–2000, the area-weighted average reconstructed temperature was higher than any other time in nearly 1,400 years.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 9
    Publication Date: 2017-07-21
    Description: Reproducible climate reconstructions of the Common Era (1 CE to present) are key to placing industrial-era warming into the context of natural climatic variability. Here we present a community-sourced database of temperature-sensitive proxy records from the PAGES2k initiative. The database gathers 692 records from 648 locations, including all continental regions and major ocean basins. The records are from trees, ice, sediment, corals, speleothems, documentary evidence, and other archives. They range in length from 50 to 2000 years, with a median of 547 years, while temporal resolution ranges from biweekly to centennial. Nearly half of the proxy time series are significantly correlated with HadCRUT4.2 surface temperature over the period 1850–2014. Global temperature composites show a remarkable degree of coherence between high- and low-resolution archives, with broadly similar patterns across archive types, terrestrial versus marine locations, and screening criteria. The database is suited to investigations of global and regional temperature variability over the Common Era, and is shared in the Linked Paleo Data (LiPD) format, including serializations in Matlab, R and Python.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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  • 10
    Publication Date: 2021-12-15
    Description: Fire plays a pivotal role in shaping terrestrial ecosystems and the chemical composition of the atmosphere and thus influences Earth’s climate. The trend and magnitude of fire activity over the past few centuries are contro- versial, which hinders understanding of preindustrial to present-day aerosol radiative forcing. Here, we present evidence from records of 14 Antarctic ice cores and 1 central Andean ice core, suggesting that historical fire activity in the Southern Hemisphere (SH) exceeded present-day levels. To understand this observation, we use a global fire model to show that overall SH fire emissions could have declined by 30% over the 20th century, possibly because of the rapid expansion of land use for agriculture and animal production in middle to high latitudes. Radiative forcing calculations suggest that the decreasing trend in SH fire emissions over the past century largely compensates for the cooling effect of increasing aerosols from fossil fuel and biofuel sources.
    Repository Name: EPIC Alfred Wegener Institut
    Type: Article , isiRev
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