TY - JOUR A1 - Lutz, C. A1 - Breuckmann, M. A1 - Hampel, S. A1 - Kreyenschmidt, M. A1 - Ke, X. A1 - Beuermann, S. A1 - Schafner, K. A1 - Turek, T. A1 - Kunz, U. A1 - de Oliveira Guilherme Buzanich, Ana A1 - Radtke, Martin A1 - Fittschen, U. E. A. T1 - Characterization of Dimeric Vanadium Uptake and Species in Nafion™ and Novel Membranes from Vanadium Redox Flow Batteries Electrolytes JF - Membranes N2 - A core component of energy storage systems like vanadium redox flow batteries (VRFB) is the polymer electrolyte membrane (PEM). In this work, the frequently used perfluorosulfonic-acid (PFSA) membrane Nafion™ 117 and a novel poly (vinylidene difluoride) (PVDF)-based Membrane are investigated. A well-known problem in VRFBs is the vanadium permeation through the membrane. The consequence of this so-called vanadium crossover is a severe loss of capacity. For a better understanding of vanadium transport in membranes, the uptake of vanadium ions from electrolytes containing Vdimer(IV–V) and for comparison also V(II), V(III), V(IV), and V(V) by both membranes was studied. UV/VIS spectroscopy, X-ray absorption near edge structure spectroscopy (XANES), total reflection X-ray fluorescence spectroscopy (TXRF), inductively coupled plasma optical emission spectrometry (ICP-OES), and micro X-ray fluorescence spectroscopy (microXRF) were used to determine the vanadium concentrations and the species inside the membrane. The results strongly support that Vdimer(IV–V), a dimer formed from V(IV) and V(V), enters the nanoscopic water-body of Nafion™ 117 as such. This is interesting, because as of now, only the individual ions V(IV) and V(V) were considered to be transported through the membrane. Additionally, it was found that the Vdimer(IV–V) dimer partly dissociates to the individual ions in the novel PVDF-based membrane. The Vdimer(IV–V) dimer concentration in Nafion™ was determined and compared to those of the other species. After three days of equilibration time, the concentration of the dimer is the lowest compared to the monomeric vanadium species. The concentration of vanadium in terms of the relative uptake λ = n(V)/n(SO3 ) are as follows: V(II) [λ = 0.155] > V(III) [λ = 0.137] > V(IV) [λ = 0.124] > V(V) [λ = 0.053] > Vdimer(IV–V) [λ = 0.039]. The results show that the Vdimer(IV–V) dimer Needs to be considered in addition to the other monomeric species to properly describe the transport of vanadium through Nafion™ in VRFBs. KW - MicroXRF KW - VRFB KW - PVDF-based membrane KW - UV/VIS KW - XANES KW - TXRF KW - ICP-OES PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-530676 DO - https://doi.org/10.3390/membranes11080576 VL - 11 IS - 8 SP - 576 PB - MDPI AN - OPUS4-53067 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Gluth, Gregor A1 - Ke, X. A1 - Vollpracht, A. A1 - Weiler, L. A1 - Bernal, S. A. A1 - Cyr, M. A1 - Dombrowski-Daube, K. A1 - Geddes, D. A. A1 - Grengg, C. A1 - Le Galliard, C. A1 - Nedeljkovic, M. A1 - Provis, J. L. A1 - Valentini, L. A1 - Walkley, B. T1 - Carbonation rate of alkali-activated concretes and high-volume SCM concretes: a literature data analysis by RILEM TC 281-CCC JF - Materials and Structures N2 - The current understanding of the carbonation and the prediction of the carbonation rate of alkali-activated concretes is complicated inter alia by the wide range of binder chemistries used and testing conditions adopted. To overcome some of the limitations of individual studies and to identify general correlations between mix design parameters and carbonation resistance, the RILEM TC 281-CCC ‘Carbonation of Concrete with Supplementary Cementitious Materials’ Working Group 6 compiled and analysed carbonation data for alkali-activated concretes and mortars from the literature. For comparison purposes, data for blended Portland cement-based concretes with a high percentage of SCMs (≥ 66% of the binder) were also included in the database. The analysis indicates that water/CaO ratio and water/binder ratio exert an influence on the carbonation resistance of alkali-activated concretes; however, these parameters are not good indicators of the carbonation resistance when considered individually. A better indicator of the carbonation resistance of alkali-activated concretes under conditions approximating natural carbonation appears to be their water/(CaO + MgOeq + Na2Oeq + K2Oeq) ratio, where the subscript ‘eq’ indicates an equivalent amount based on molar masses. Nevertheless, this ratio can serve as approximate indicator at best, as other parameters also affect the carbonation resistance of alkali-activated concretes. In addition, the analysis of the database points to peculiarities of accelerated tests using elevated CO2 concentrations for low-Ca alkali-activated concretes, indicating that even at the relatively modest concentration of 1% CO2, accelerated testing may lead to inaccurate predictions of the carbonation resistance under natural exposure conditions. KW - Alkali-activated materials KW - Durability KW - Carbonation KW - Accelerated testing PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-560037 DO - https://doi.org/10.1617/s11527-022-02041-4 VL - 55 IS - 8 SP - 1 EP - 15 PB - Springer Nature AN - OPUS4-56003 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gluth, Gregor A1 - Ke, X. A1 - Vollpracht, A. A1 - Bernal, S. A. A1 - Cizer, Ö. A1 - Cyr, M. A1 - Dombrowski-Daube, K. A1 - Geddes, D. A1 - Grengg, C. A1 - Le Galliard, C. A1 - Nedeljkovic, M. A1 - Provis, J. L. A1 - Shi, Z. A1 - Valentini, L. A1 - Walkley, B. ED - Escalante-Garcia, J. I. ED - Castro Borges, P. ED - Duran-Herrera, A. T1 - RILEM TC 281-CCC Working Group 6: Carbonation of alkali activated concrete—preliminary results of a literature survey and data analysis T2 - Proceedings of the 75th RILEM Annual Week 2021: Advances in Sustainable Construction Materials and Structures N2 - The current understanding of the carbonation of alkali-activated concretes is ham-pered inter alia by the wide range of binder chemistries used. To overcome some of the limitations of individual studies and to identify general correlations between their mix design parameters and carbonation resistance, the RILEM TC 281-CCC working group 6 compiled carbonation data for alkali-activated concretes and mortars from the literature. For comparison purposes, data for blended Portland cement-based concretes with a high percentage of SCMs (≥ 66 % of the binder) were also included in the database. A preliminary analysis of the database indicates that w/CaO ratio and w/b ratio exert an influence on the carbonation resistance of alkali-activated concretes but, contrary to what has been reported for concretes based on (blended) Portland cements, these are not good indicators of their carbonation resistance when considered individually. A better indicator of the carbonation resistance of alkali-activated concretes under conditions approxi-mating natural carbonation appears to be their w/(CaO + Na2O + K2O) ratio. Furthermore, the analysis points to significant shortcomings of tests at elevated CO2 concentrations for low-Ca alkali-activated concretes, indicating that even at a concentration of 1 % CO2, the outcomes may lead to inaccurate predictions of the carbonation coefficient under natural exposure conditions. T2 - 75th RILEM Annual Week CY - Mérida, Yucatán, Mexico DA - 30.08.2021 KW - Alkali-activated materials KW - Durability KW - Carbonation KW - Testing KW - Concrete PY - 2023 SN - 978-3-031-21734-0 SN - 978-3-031-21735-7 DO - https://doi.org/10.1007/978-3-031-21735-7_72 SN - 2211-0852 SN - 2211-0844 VL - 40 SP - 667 EP - 676 PB - Springer CY - Cham AN - OPUS4-57157 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Lutz, C. A1 - Hampel, S. A1 - Ke, X. A1 - Beuermann, S. A1 - Turek, T. A1 - Kunz, U. A1 - de Oliveira Guilherme Buzanich, Ana A1 - Radtke, Martin A1 - Fittschen, U. T1 - Evidence for redox reactions during vanadium crossover inside the nanoscopic water-body of Nafion 117 using X-ray absorption near edge structure spectroscopy JF - Journal of Power Sources N2 - A major source of capacity fade of the common vanadium redox flow battery (VRFB) is the vanadium ion transport through the separator. However, different transport models disagree significantly in the diffusion coefficient for the different V species and the influence of different transport mechanisms. The underlying hypothesis of this work is that reactions inside the membrane are partly responsible for these discrepancies. Accordingly, it was investigated if redox reactions inside the nanoscopic water body of Nafion 117 can occur. X-ray absorption near edge structure spectroscopy (XANES) was used to distinguish between the different V species inside hydrated Nafion 117 and novel PVDF-based membranes. It was validated that the speciation of vanadium can be performed using the pre-edge peak energy and intensity. The experiments were performed as follows: strips of the membrane were exposed from one site to a V3+ solution (green) and from the other site to a VO2+ solution (yellow). The ions could diffuse into the membrane from both sides. A change of color of the membrane strip was observed. The blue color in the middle of the strip indicated that VO2+ was formed where V3+ and VO2+ got in contact. Using XANES this reaction inside Nafion was proven. KW - PVDF-Based membrane KW - VRFB KW - Vanadium speciation KW - XANES KW - Nafion 117 PY - 2020 DO - https://doi.org/10.1016/j.jpowsour.2020.229176 VL - 483 SP - 229176 PB - Elsevier B.V. AN - OPUS4-51719 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Vogel, F. A1 - Cheng, J. A1 - Liang, S. B. A1 - Ke, C. B. A1 - Cao, S. S. A1 - Zhang, X. P. A1 - Zizak, I. A1 - Manzoni, Anna Maria A1 - Yu, J. M. A1 - Wanderka, N. A1 - Li, W. T1 - Formation and evolution of hierarchical microstructures in a Ni-based superalloy investigated by in situ high-temperature synchrotron X-ray diffraction JF - Journal of alloys and compounds N2 - Hierarchical microstructures are created when additional γ particles form in γ’ precipitates and they are linked to improved strength and creep properties in high-temperature alloys. Here, we follow the formation and evolution of a hierarchical microstructure in Ni86.1Al8.5Ti5.4 by in situ synchrotron X-ray diffraction at 1023 K up to 48 h to derive the lattice parameters of the γ matrix, γ’ precipitates and γ particles and misfits between phases. Finite element method-based computer simulations of hierarchical microstructures allow obtaining each phase's lattice parameter, thereby aiding peak identification in the in situ X-ray diffraction data. The simulations further give insight into the heterogeneous strain distribution between γ’ precipitates and γ particles, which gives rise to an anisotropic diffusion potential that drives the directional growth of γ particles. We rationalize a schematic model for the growth of γ particles, based on the Gibbs-Thomson effect of capillary and strain-induced anisotropic diffusion potentials. Our results highlight the importance of elastic properties, elastic anisotropy, lattice parameters, and diffusion potentials in controlling the behavior and stability of hierarchical microstructures. KW - XRD KW - Superalloy KW - Finite element method KW - Transmission electron microscopy PY - 2022 DO - https://doi.org/10.1016/j.jallcom.2022.165845 SN - 0925-8388 VL - 919 SP - 1 EP - 17 PB - Elsevier CY - Lausanne AN - OPUS4-55394 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Gluth, Gregor A1 - Ke, X. A1 - Vollpracht, A. A1 - Weiler, L. A1 - Bernal, S. A. A1 - Cyr, M. A1 - Dombrowski-Daube, K. A1 - Geddes, D. A1 - Grengg, C. A1 - Le Galliard, C. A1 - Nedeljkovic, M. A1 - Provis, J. L. A1 - Valentini, L. A1 - Walkley, B. ED - Jędrzejewska, A. ED - Kanavaris, F. ED - Azenha, M. ED - Benboudjema, F. ED - Schlicke, D. T1 - Carbonation of alkali-activated concretes: effects of compositional parameters and carbonation conditions T2 - International RILEM Conference on Synergising Expertise towards Sustainability and Robustness of Cement-based Materials and Concrete Structures: SynerCrete 2023 N2 - The current ability to predict the carbonation resistance of alkali-activated materials (AAMs) is incomplete, partly because of widely varying AAM chemistries and variable testing conditions. To identify general correlations between mix design parameters and the carbonation rate of AAMs, RILEM TC 281-CCC Working Group 6 compiled and analysed carbonation data for alkali-activated concretes and mortars from the literature. For comparison purposes, data for blended Portland cement-based concretes with a high percentage of SCMs (≥66% of the binder) were also included in the database. The results show that the water/CaO ratio is not a reliable indicator of the carbonation rate of AAMs. A better indicator of the carbonation rate of AAMs under conditions approximating natural carbonation is their water/(CaO + MgOeq + Na2Oeq + K2Oeq) ratio, where the index ‘eq’ indicates an equivalent amount based on molar masses. This finding can be explained by the CO2 binding capacity of alkaline-earth and alkali metal ions; the obtained correlation also indicates an influence of the space-filling capability of the binding phases of AAMs, as for conventional cements. However, this ratio can serve only as an approximate indicator of carbonation resistance, as other parameters also affect the carbonation resistance of alkali-activated concretes. In addition, the analysis of the dataset revealed peculiarities of accelerated tests using elevated CO2 concentrations for low-Ca AAMs, indicating that even at the relatively modest concentration of 1% CO2, accelerated testing may lead to inaccurate predictions of their carbonation resistance under natural exposure conditions. T2 - International RILEM Conference on Synergising Expertise towards Sustainability and Robustness of Cement-based Materials and Concrete Structures: SynerCrete 2023 CY - Adamantas, Greece DA - 14.06.2023 KW - Carbonation KW - Alkali-activated materials KW - Mix design PY - 2023 DO - https://doi.org/10.1007/978-3-031-33187-9_94 VL - 2 SP - 1029 EP - 1037 PB - Springer CY - Cham AN - OPUS4-57699 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -