TY - JOUR A1 - Gnutzmann, Tanja A1 - Nguyen, Thi Yen A1 - Rademann, K. A1 - Emmerling, Franziska T1 - Solvent-triggered crystallization of polymorphs studied in situ N2 - The crystallization of a highly polymorphic compound was studied in situ by combined time-resolved X-ray diffraction and Raman spectroscopy. Any influences of solid surfaces, temperature, and humidity on the crystallization were omitted by the use of a specially designed acoustic levitator. Investigations of polymorphic phase transitions during the crystallization process in different solvents allowed a structure assignment from first crystalline assemblies to final crystalline form. For the first time, it was possible to yield pure phases of selected polymorphs of the model compound ROY (5-methyl-2-[(2-nitrophenyl)amino]-3-thiophenecarbonitrile) directly from solution. The influence of the solvent on the final products and transient phases during the crystallization process was elucidated. KW - Polymorphism KW - Crystallization KW - In situ WAXS KW - In situ Raman spectroscopy KW - ROY PY - 2014 DO - https://doi.org/10.1021/cg501287v SN - 1528-7483 VL - 14 IS - 12 SP - 6445 EP - 6450 PB - American Chemical Society CY - Washington, DC, USA AN - OPUS4-32583 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Goedecke, Caroline A1 - Sojref, Regine A1 - Nguyen, Thi Yen A1 - Piechotta, Christian T1 - Immobilization of photocatalytically active TiO2 nanopowder by high shear granulation N2 - Nano-TiO2 powder is known to show high photocatalytic reactivity in the degradation of several organic pollutants. In thiswork, the powderwas fixed on the surface of SiO2 granuleswith the size of several micrometers using a high shear granulation process. Nanozirconia sol was applied as an inorganic binder. When the samples were tempered at 300 °C, they showed high stability in an aqueous solution for several hours. An energy dispersive x-ray spectroscopy (EDX) analysis confirmed that the cores and shells of the granules consisted solely of SiO2 and TiO2 respectively, and that ZrO2 was found throughout the whole granules. Methylene blue (MB) was employed as amodel systemto evaluate the photocatalytic activity of the TiO2 nanopowder and coated granules. Itwas shown that the TiO2-coated granules lead to the degradation ofMB under UV irradiation,whereas no effect was observed in the dark. After the Degradation experiments the granules could be recovered and they remained active for further applications. KW - Heterogeneous photocatalysis KW - Water treatment KW - Advanced oxidation KW - Nanozirconia KW - Methylene blue PY - 2017 DO - https://doi.org/10.1016/j.powtec.2017.06.025 SN - 0032-5910 SN - 1873-328X VL - 318 SP - 465 EP - 470 AN - OPUS4-41608 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Batzdorf, Lisa A1 - Nguyen, Thi Yen A1 - Rump, Doreen A1 - Emmerling, Franziska T1 - Crystallization behavior of carbamazepine N2 - Carbamazepine (CBZ) is known for its variety of anhydrous and hydrous polymorphs. Herein, a thorough analysis of the crystallization behavior of CBZ is presented. The influence of the solvent and the concentration on the crystallization behavior under different environmental conditions is investigated by combined in situ XRD and Raman spectroscopy measurements. Crystallization studies conducted via conventional crystallization in glass tubes and in levitated droplets using an acoustic levitator indicate a dependence of the crystallization process from solvent and surface. KW - Carbamazepine KW - Polymorphism KW - Acoustic levitation KW - XRD KW - Raman spectroscopy PY - 2014 DO - https://doi.org/10.1515/zpch-2013-0452 SN - 0942-9352 SN - 2196-7156 SN - 0044-3336 SN - 0044-3328 SN - 0942-9352 N1 - Geburtsname von Batzdorf, Lisa: Tröbs, L. - Birth name of Batzdorf, Lisa: Tröbs, L. VL - 228 IS - 4-5 SP - 493 EP - 501 PB - Oldenbourg CY - München AN - OPUS4-30627 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - In situ characterization of crystallization processes T2 - BESSY Usermeeting 2013 CY - Berlin, Germany DA - 2013-12-05 PY - 2013 AN - OPUS4-30022 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - In-situ-Charakterisierung der Kristallisation organischer Polymorphe T2 - Workshop "Zeit- und temperaturaufgelöste Röntgen-Pulver-Diffraktometrie CY - Pfinztal, Germany DA - 2013-11-14 PY - 2013 AN - OPUS4-29830 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Joseph, A. A1 - Bernardes, C. E. S. A1 - Druzhinina, A. I. A1 - Varushchenko, R. M. A1 - Nguyen, Thi Yen A1 - Emmerling, Franziska A1 - Yuan, L. A1 - Dupray, V. A1 - Coquerel, G. A1 - Minas da Piedade, M. E. T1 - Polymorphic phase transition in 4′-hydroxyacetophenone: Equilibrium temperature, kinetic barrier, and the relative stability of Z′=1 and Z′=2 forms N2 - Particularly relevant in the context of polymorphism is understanding how structural, thermodynamic, and kinetic factors dictate the stability domains of polymorphs, their tendency to interconvert through phase transitions, or their possibility to exist in metastable states. These three aspects were investigated here for two 4′-hydroxyacetophenone (HAP) polymorphs, differing in crystal system, space group, and number and conformation of molecules in the asymmetric unit. The results led to a ΔfGm°-T phase diagram highlighting the enantiotropic nature of the system and the fact that the Z′=1 polymorph is not necessarily more stable than its Z′=2 counterpart. It was also shown that the form II → form I transition is entropy driven and is likely to occur through a nucleation and growth mechanism, which does not involve intermediate phases, and is characterized by a high activation energy. Finally, although it has been noted that conflicts between hydrogen bond formation and close packing are usually behind exceptions from the hypothesis of Z′=1 forms being more stable than their higher Z′ analogues, in this case, the HAP polymorph with stronger hydrogen bonds (Z′=2) is also the one with higher density. KW - Polymorphism KW - Polymorphic transition KW - 4'-hydroxyacetophenone PY - 2017 DO - https://doi.org/10.1021/acs.cgd.6b01876 SN - 1528-7483 SN - 1528-7505 VL - 17 IS - 4 SP - 1918 EP - 1932 PB - ACS AN - OPUS4-40167 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Nguyen, Thi Yen A1 - Roessler, Ernst A1 - Rademann, Klaus A1 - Emmerling, Franziska T1 - Control of organic polymorph formation: crystallization pathways in acoustically levitated droplets N2 - Theoretical and experimental studies indicate that crystal nucleation can take more complex pathways than expected on the ground of the classical nucleation theory. Among these pathways are the formation of pre-nucleation clusters and amorphous precursor phases. A direct in situ observation of the different pathways of nucleation from solution is challenging since the paths can be influenced by heterogeneous nucleation sites, such as container walls. Here, we provide insights into the crystallization process using the in situ combination of an acoustic levitator, Raman spectroscopy, and X-ray scattering. The contactless sample holder enables the observation of homogeneous crystallization processes and the detection of intermediates and final crystalline forms. We provide evidence for the existence of multiple pathways of nucleation based on the investigation of the crystallization of organic molecules from different solvents. Starting from a diluted solution, a supersaturation is reached during the experiment due to the evaporation of the solvent. The highly supersaturated solution reveals different pathways of crystallization. Depending on the degree of supersaturation either the thermodynamically stable or the metastable crystal form is observed. KW - Crystallization KW - In situ XRD KW - Polymorphism KW - Polyamorphism KW - Raman spectroscopy PY - 2017 DO - https://doi.org/10.1515/zkri-2016-1964 SN - 2194-4946 SN - 2196-7105 VL - 232 IS - 1-3 SP - 15 EP - 24 PB - De Gruyter CY - Berlin AN - OPUS4-39708 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Nguyen, Thi Yen A1 - Rademann, K. A1 - Emmerling, Franziska T1 - Direct evidence of polyamorphism in paracetamol N2 - While polymorphism is a common phenomenon in the crystallization processes of organic compounds, polyamorphism has gained importance only recently. Using sophisticated sample environments and applying in situ scattering methods and vibrational spectroscopy, the complete crystallization process of organic compounds from solution can be traced and characterized. Diffuse scattering from amorphous intermediates can be investigated by analyzing the atomic pair distribution function (PDF) to gain further insights into molecular pre-orientation. The crystallization behavior of paracetamol was studied exemplarily under defined, surface-free conditions. Based on the choice of the solvent, the formation of different polymorphs is promoted. The thermodynamically stable form I and the metastable orthorhombic form II could be isolated in pure form directly from solution. For both polymorphs, the crystallization from solution proceeds via a distinct amorphous precursor phase. PDF analyses of these different amorphous states indicate a specific pre-orientation of the analyte molecules introduced by the solvent. The resulting crystalline polymorph is already imprinted in these proto-crystalline precursors. Direct experimental evidence for the polyamorphism of paracetamol is provided. PY - 2015 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-351366 DO - https://doi.org/10.1039/C5CE01583A SN - 1466-8033 VL - 17 IS - 47 SP - 9029 EP - 9036 PB - Royal Society of Chemistry CY - London, UK AN - OPUS4-35136 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Stroh, Julia A1 - Schlegel, Moritz-Caspar A1 - Schmidt, Wolfram A1 - Nguyen, Thi Yen A1 - Meng, Birgit A1 - Emmerling, Franziska T1 - Time-resolved in situ investigation of Portland cement hydration influenced by chemical admixtures N2 - 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. KW - Synchrotron KW - Portland cement Initial hydration KW - Superplasticizer KW - Stabilizer KW - XRD PY - 2016 DO - https://doi.org/http://dx.doi.org/10.1016/j.conbuildmat.2015.12.097 IS - 106 SP - 18 EP - 26 PB - Elsevier AN - OPUS4-35467 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - Guided crystallization: The influence of solvent and concentration N2 - Theoretical and experimental studies indicate that crystal nucleation can take more complex pathways than expected on the ground of the classical nucleation theory. A direct in situ observation of the different pathways of nucleation from solution is challenging since the paths can be influenced by heterogeneous nucleation sites, such as container walls. The custom-made acoustic levitator using in these experiments regulates the influence that solid surfaces, temperature, and humidity have on the crystallization process. The investigations of the crystallization process of paracetamol were performed with in situ analytical techniques and theoretical simulations to gain a comprehensive insight into processes, occurring intermediates, and required reaction conditions. The targeted choice of the solvent and the concentration enabled the guidance of the pathways, therefore, resulting in the isolation of one desired crystalline structure. T2 - Annual COST meeting CY - Lincoln, United Kingdom DA - 25.06.2017 KW - Crystallization KW - Polymorphism KW - Molecular dynamic simulation KW - Pair distribution function analysis KW - XRD PY - 2017 AN - OPUS4-41111 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - Paracetamol: Polymorphs and Intermediates T2 - BESSY Usermeeting 2015 CY - Berlin-Adlershof, Germany DA - 2015-12-10 PY - 2015 AN - OPUS4-35260 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - Paracetamol: Polymorphs and Intermediates T2 - COST Summer-School 2015 CY - Berlin-Adlershof, Germany DA - 2015-11-23 PY - 2015 AN - OPUS4-35261 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - Desolvation of indometacin solvates characterized structurally and kinetically N2 - The structure of indometacin solvates and the desolvation process of these compounds are investigated by synchrotron X-ray radiation, Raman spectroscopy and thermal analysis. T2 - Annual CM1402 crystallize COST meeting CY - Coimbra, Portugal DA - 06.04.2016 KW - Crystallization KW - In situ analysis KW - Indometacin KW - Active pharmaceutical ingredient (API) PY - 2016 AN - OPUS4-35872 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Nguyen, Thi Yen T1 - Direct evidence of polyamorphism in paracetamol N2 - While polymorphism is a common phenomenon in the crystallization processes of organic compounds, polyamorphism has gained importance only recently. Using sophisticated sample environments and applying in situ scattering methods and vibrational spectroscopy, the complete crystallization process of organic compounds from solution can be traced and characterized. Diffuse scattering from amorphous intermediates can be investigated by analyzing the atomic pair Distribution function (PDF) to gain further insights into molecular pre-orientation. The crystallization behavior of Paracetamol was studied exemplarily under defined, surface-free conditions. Based on the choice of the solvent, the formation of different polymorphs is promoted. The thermodynamically stable form I and the metastable orthorhombic form II could be isolated in pure form directly from solution. For both polymorphs, the crystallization from solution proceeds via a distinct amorphous precursor phase. PDF analyses of these different amorphous states indicate a specific pre-orientation of the analyte molecules introduced by the solvent. The resulting crystalline polymorph is already imprinted in these proto-crystalline precursors. Direct experimental evidence for the polyamorphism of paracetamol is provided. T2 - Annual CM1402 crystallize COST meeting CY - Coimbra, Portugal DA - 06.04.2016 KW - Paracetamol KW - Crystallization KW - In situ analysis KW - Active pharmaceutical ingredient (API) PY - 2016 AN - OPUS4-35873 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -