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      • Biophysical and economic limits to negative CO<sub>2</sub> emissions

        Smith, Pete,Davis, Steven J.,Creutzig, Felix,Fuss, Sabine,Minx, Jan,Gabrielle, Benoit,Kato, Etsushi,Jackson, Robert B.,Cowie, Annette,Kriegler, Elmar,van Vuuren, Detlef P.,Rogelj, Joeri,Ciais, Philipp Nature Publishing Group 2016 Nature climate change Vol.6 No.1

        <P>To have a >50% chance of limiting warming below 2 degrees C, most recent scenarios from integrated assessment models (IAMs) require large-scale deployment of negative emissions technologies (NETs). These are technologies that result in the net removal of greenhouse gases from the atmosphere. We quantify potential global impacts of the different NETs on various factors (such as land, greenhouse gas emissions, water, albedo, nutrients and energy) to determine the biophysical limits to, and economic costs of, their widespread application. Resource implications vary between technologies and need to be satisfactorily addressed if NETs are to have a significant role in achieving climate goals.</P>

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        New insights in the formation processes of Pu(IV) colloids

        Walther, Clemens,Rothe, Jö,rg,Brendebach, Boris,Fuss, Markus,Altmaier, Marcus,Marquardt, Christian M.,,chner, Sebastian,Cho, Hye-Ryun,Yun, J.-I.,Seibert, Alice De Gruyter Oldenbourg 2009 RADIOCHIMICA ACTA Vol.97 No.4

        <P><B>Abstract</B></P><P>The high tendency of tetravalent plutonium to form polymeric complexes and colloids is well known but the exact processes underlying their formation are still controversially discussed. In the present work, the nucleation of small polynuclear hydroxide complexes,<I>i.e.</I>, ionic species containing more than one Pu ion, their aggregation and formation of larger colloids (polymers exceeding some 5 nm in size) and finally ripening processes of freshly formed amorphous Pu(IV) colloids towards more crystalline particles are investigated by use of a combination of various spectroscopic techniques. By electrospray mass-spectrometry small polymers such as dimers, trimers and tetramers containing mixed oxidation states of Pu were observed. These polymers might be responsible for the equilibration between the Pu(III)/Pu(IV) and the plutonyl species Pu(V)/Pu(VI) even in dilute solutions in the absence of colloids or precipitates.</P>

      • Chemical Behavior of Niobium(V) in Cementitious Conditions: Solubility and Sorption

        Yongheum Jo,Nese Cevirim-Papaioannou,Krassimir Garbev,Markus Fuss,Karsten Franke,Oliver Dieste Blanco,Benny de Blochouse,Marcus Altmaier,Xavier Gaona 한국방사성폐기물학회 2022 한국방사성폐기물학회 학술논문요약집 Vol.20 No.2

        Niobium (Nb) is present in Ni-based alloys and stainless steels used in nuclear reactors as structural materials. Nb-93 is a naturally occurring and stable isotope of niobium and Nb-94 (half-life = 20,000 years) is produced by neutron activation of Nb-93. Nb-94 can be present in waste streams from dismantling of nuclear power plants and treatment of the primary coolant circuit. Hence, the radioactive wastes containing active Nb-94 are disposed of in the repositories for low- and intermediate-level waste (LILW). Nb predominantly exhibits a pentavalent oxidation state (i.e., +V) within the stability field of water. Cementitious materials (concrete, mortar, and grout) are extensively utilized in LILW disposal systems as structural components and chemical agents for the stabilization of waste. Solubility defines the source term (i.e., upper concentration limit) in the repository system. However, the solubility behavior of Nb in cementitious systems at high pH remains ill-defined, and information available on the Nb solid phases controlling the solubility is scarce and often ambiguous. Sorption on cementbased materials is one of the main mechanisms controlling the retention of niobium(V) in a LILW repository, and distribution coefficients (Rd) are necessary to evaluate the retention capacity by sorption in the safety assessment of disposal systems. Available sorption data of Nb(V) on cement showed a large discrepancy in Rd, moreover, no sorption data is available for Nb(V) under conditions characterizing the first degradation stage of cement (young cement condition) at pH 13 – 13.5. In this context, the solubility of Nb was extensively investigated in porewater conditions representative of the cement degradation stage I, as well as in CaCl2-Ca(OH)2 systems. Special focus was given to the accurate characterization of the solubility-controlling solid niobium phases. We also studied the sorption of Nb(V) by hardened cement pastes (HCP) and calcium silicate hydrates (CSH, major hydrate of HCP). This work provides the results on Rd, sorption isotherm and sorption mechanisms of Nb(V). Besides, the impact of ISA (polyhydroxycarboxylic acid generated by the degradation of cellulose) on Nb(V) sorption and the dissolution of cement materials was investigated.

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