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- 2016 (4) (entfernen)
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- Hydrogen storage (1)
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- Portland cement Initial hydration (1)
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Eingeladener Vortrag
- nein (2)
We have studied the mechanism of hydrogen storage in the aluminium based metal–organic framework CAU-1 or [Al4(OH)2 OCH3)4(O2C-C6H3NH2-CO2)3] using a complementary multidisciplinary approach of volumetric gas sorption analysis, in situ neutron diffraction and spectroscopy and ab initio calculations. The structure of CAU-1 forms two different types of microporous cages: (i) an octahedral cage with a diameter of about 10 Å and (ii) a tetrahedral cage with a diameter of about 5 Å. Though all metal sites of CAU-1 are fully coordinated, the material exhibits relatively high storage capacities, reaching 4 wt% at a temperature of 70 K. Our results reveal that hydrogen sorption is dominantly driven by cooperative guest–guest interactions and interactions between guest hydrogen molecules and organic linkers. The adsorption of hydrogen on the organic linkers leads to the contraction of the host framework structure and as a result to changes in the electronic potential surface inside the pores. This, in turn, leads to cooperative rearrangement of the molecules inside the pores and to the formation of additionally occupied positions, increasing hydrogen uptake. At the final stage we observe the formation of solid amorphous hydrogen inside the pores.
Time-resolved in situ investigation of Portland cement hydration influenced by chemical admixtures
(2016)
Numerous admixtures are used in the building practice to customize the properties of the cement paste during application. The influences of admixtures on the course of cement hydration and formation of hydrate phases have to be considered. Polycarboxylate ether (PCE) based polymeric superplasticizers (SPs) are known to retard the setting of the cement paste. The extent of the retardation differs depending on the molecular structure of the SP. Additionally, the presence of a stabilizing agent (SA) in the cement paste has a retarding side effect on the setting. The initial cement hydration processes and the detailed mechanisms of the retardation influenced by PCEs, as well as their interactions with particular SAs, are insufficiently understood. Up to now, only the results of phenomenological studies were taken into account to describe this retardation process. A detailed structure analysis monitoring the change of the phase composition during the hydration was never applied. Both SP and SA affect the adsorption of the sulphate ions on the clinker particles, causing changes in the formation of ettringite during the initial hydration, and are therefore a crucial part of the setting process itself. Here, the initial hydration of cement influenced by the interaction of SP and SA was monitored in situ by synchrotron X-ray diffraction. The high time resolution of the measurements allowed a continuous detection of the hydrates formed. The hydration was followed from the starting point of water addition and for couple of hours afterwards. The hydration of the levitated cement pellets containing starch as SA was initialized by adding aqueous solutions of different commercial SPs. Changes in the ettringite formation were detected in comparison to the reference hydration of pure cement.