Collaborative Research Center/Transregio 63
"Integrated Chemical Processes in Liquid Multiphase Systems"
"Integrated Chemical Processes in Liquid Multiphase Systems"
Collaborative Research Center/Transregio 63
"Integrated Chemical Processes in Liquid Multiphase Systems"
Sub-Coordinators: Prof. Dr.-Ing. Anja Drews Prof. Dr. Regine von Klitzing
Researchers: M. Sc. Sebastian Stock, M. Sc. Maresa Kempin
B6 aims at developing and evaluating separation und switching strategies for Pickering emulsions (PE) in liquid/liquid (L/L) reactions. PEs will be optimized to yield high conversion in the reductive amination of aldehydes and at the same time high separation efficiency.
Concepts developed in the 2nd funding period for the hydroformylation of dodecene will be adapted and expanded.
In contrast to hydroformylation, the new challenge is the need of removing the water produced by amination. Different strategies will be investigated, e.g.:
Besides investigating the influence of operating conditions on the permeability of the different w/o and o/w PE, a deeper understanding of phenomena occurring near the membrane will be gained by direct observation of the deposit layer. This will be required for mechanistic modelling and to explain the observed increase in permeability (see Fig.).
In addition, B6 will develop a micellar enhanced ultrafiltration (MEUF) step for the recycle of surfactants and catalyst from the decanted water phase in MLS which will later be integrated into the miniplant (with D2).
Figure 1: Disproportionate flux increase [Skale et al., J. Membr. Sci. 535 (2017) 1-9]
A2 (Schomäcker): Influence of catalyst ligand complexes, network analysis of total and sub reaction networks, evaluation of catalyst deactivation
A9 (Enders, Sadowski): Solubilization of weakly polar compounds in micellar systems
A10 (Böhm, Hecht, Kraume): Gas/Liquid Mass Transfer in Reactive Multiphase Systems
B8 (Kraume, Thévenin): Characterization, modeling and simulation of phase separation in micellar multiphase systems
D1 (Engell, Sadowski, Sundmacher): Fast model-based design of chemical processes with several liquid phases
D2 (Repke): Demonstration of the Fast Track Process Development and of the Optimal Operation of the Reductive Amination of Long-chained Aldehydes in Emulsion Systems
Stock, S.; von Klitzing, R. Microgels at Droplet Interfaces of Water-in-Oil Emulsions - Challenges and Progress. Current Opinion in Colloid & Interface Science, 58, 101561, 2022. [DOI:10.1016/j.cocis.2021.101561]
Kempin, M. V.; Drews, A. What Governs Pickering Emulsion Properties During Preparation via Batch Rotor‐Stator Homogenizers? Chem. Ing. Tech. 93 (1–2), 311-317, 2021. [doi.org/10.1002/cite.202000130]
Kempin, M. V.; Drews A. Organic Solvent Nanofiltration of Water-in-Oil Pickering Emulsions - What Influences Permeability? Membranes, 11, 864, 2021. [DOI:10.3390/membranes11110864]
Stock, S.; Jakob, F.; Röhl, S.; Gräff, K.; Kühnhammer, M.; Hondow, N.; Micklethwaite, S.; Kraume, M.; von Klitzing, R. Exploring Water in Oil Emulsions simultaneously stabilized by solid hydrophobic Silica Nanospheres and hydrophilic soft PNIPAM Microgel. Soft matter 17, 8258–8268, 2021. [DOI:10.1039/D1SM00942G]
Stock, S.; Schlander, A.; Kempin, M.; Geisler, R.; Stehl, D.; Spanheimer, K.; Hondow, N.; Micklethwaite, S.; Weber, A.; Schomäcker, R.; Drews, A.; Gallei, M.; von Klitzing, R.The quantitative impact of fluid vs. solid interfaces on the catalytic performance of pickering emulsions, Phys. Chem. Chem. Phys., 23, 2355-2367, 2021. [DOI:10.1039/D0CP06030E]
Kempin, M.V.; Kraume, M.; Drews, A. W/O Pickering emulsion preparation using a batch rotor-stator mixer - influence on rheology, drop size distribution and filtration behavior, J. Coll. Interf. Sci 573, 135-149, 2020. [doi.org/10.1016/j.jcis.2020.03.103]
Kempin, M.V.; Stock, S.; von Klitzing R.; Kraume, M.; Drews, A. Influence of particle type and concentration on the ultrafiltration behavior of nanoparticle stabilized Pickering emulsions and suspensions. Separation and Purification Technology, 252, 117457, 2020. [doi.org/10.1016/j.seppur.2020.117457]
Stehl, D.; Skale, T.; Hohl, L.; Lvov, Y.; Koetz,J.; Kraume,M.; Drews, A.; von Klitzing. R. Oil-in-Water Pickering Emulsions Stabilized by Halloysite Clay Nanotubes Toward Efficient Filterability. ACS Applied Nano Materials. 3, 12, 11743–11751, 2020. [DOI: 10.1021/acsanm.0c02205]
Röhl, S ; Hohl, L.; Kempin, M.; Enders, F.; Jurtz, N.; Kraume, M. Influence of Different Silica Nanoparticles on Drop Size Distributions in Agitated Liquid‐Liquid Systems. Chem. Ing. Tech. 91, No. 11, 1640–1655, 2019. [ doi.org/10.1002/cite.201900049]
Stehl, D.; Milojević, N.; Stock, S.; Schomäcker, R.; von Klitzing, R. Synergistic Effects of Rh-catalyst on Particle Stabilized Pickering Emulsions for Hydroformylation of Long Chain Olefins. Industrial & Engineering Chemistry Research, 58(7), 2524-2536, 2019, [DOI: 10.1021/acs.iecr.8b04619]
Bibouche, B.; Peral, D.; Stehl, D.; Söderholm, V.; Schomäcker, R.; von Klitzing, R.; Vogt, D. Multiphasic aqueous hydroformylation of 1-alkenes with micelle-like polymer particles as phase transfer agents. RSC Adv., 8, 23332-23338, 2018. [doi:10.1039/C8RA04022B]
Peral, D.; Stehl, D.; Bibouche, B.; Yu, H.; Mardoukh, J.; Schomacker, R.; von Klitzing, R.; Vogt, D. Colloidal polymer particles as catalyst carriers and phase transfer agents in multiphasic hydroformylation reactions. J. Colloid Interface Sci., 513, 647-657. 2018. [doi.org/10.1016/j.jcis.2017.11.071]
Petzold, M.; Rohl, S.; Hohl, L.; Stehl, D.; Lehmann, M.; von Klitzing, R.; Kraume, M. Mass Transfer and Drop Size Distributions in Reactive Nanoparticle-Stabilized Multiphase Systems. Chem. Ing. Tech., 89(11), 1561-1573, 2017. [doi: 10.1002/cite.201700060]
Skale, T.; Hohl, L.; Kraume, M.; Drews, A. Feasibility of w/o Pickering emulsion ultrafiltration. J. Membr. Sci ., 535, 1-9, 2017. [doi.org/10.1016/j.memsci.2017.04.006]
Von Klitzing, R.; Stehl, D.; Pogrzeba, T.; Schomäcker, R.; Minullina, R.; Panchal, A.; Konnova, S.; Fakhrullin, R. Koetz, J.; Möhwald, H.; Lvov, Y. Halloysites Stabilized Emulsions for Hydroformylation of Long Chain Olefins. Adv. Mater. Interfaces, 4(1), 1600435, 2017. [doi: 10.1002/admi.201600435]
Zedel, D.; Kraume, M.; Drews, A. Modelling and prediction of organic solvent flux and retention of surfactants by organic solvent nanofiltration. J. Membr. Sci., 544, 323-332, 2017. [doi: https://doi.org/10.1016/j.memsci.2017.09.041]
Hohl, L.; Röhl, S.; Stehl, D.; von Klitzing, R.; Kraume, M. Influence of Nanoparticles and Drop Size Distributions on the Rheology of w/o Pickering Emulsions. Chem. Ing. Tech., 88(11), 1815-1826, 2016. [doi:10.1002/cite.201600063]
Schmidt, M.; Pogrezba, T.; Stehl, D.; Sachse, R.; Schwarze, M.; von Klitzing, R.; Schomäcker, R. Verteilungsgleichgewichte von Liganden in mizellaren Lösungsmittelsystemen. Chem. Ing. Tech., 88(1-2), 119–127, 2016. [doi:10.1002/cite.201500125]
Skale, T.; Stehl, D.; Hohl, L.; Kraume, M.; von Klitzing, R.; Drews, A. Tuning Pickering Emulsions for Optimal Reaction and Filtration Conditions. Chem. Ing. Tech., 88(11), 1827-1832, 2016. [doi: 10.1002/cite.201600099]
Stehl, D.; Hohl, L.; Schmidt, M.; Hübner, J.; Lehmann, M.; Kraume, M.; Schomäcker, R.; von Klitzing, R. Characteristics of Stable Pickering Emulsions under Process Conditions. Chem. Ing. Tech., 88(11), 1806-1814, 2016. [doi: 10.1002/cite.201600065]
Von Klitzing, R.; Stehl, D.; Pogrzeba, T.; Schomäcker, R.; Minullina, R.; Panchal, A.; Konnova, S.; Fakhrullin, R. Koetz, J.; Möhwald, H.; Lvov, Y. Halloysites Stabilized Emulsions for Hydroformylation of Long Chain Olefins. Adv. Mater. Interfaces, 2016. [doi: 10.1002/admi.201600435]
Zedel, D.; Drews, A.; Kraume, M. Retention of surfactants by organic solvent nanofiltration and influences on organic solvent flux. Sep. Purif. Technol., 158, 396–408, 2016. [doi:10.1016/j.seppur.2015.12.040]
Carl, A.; Bannuscher, A.; von Klitzing, R. Particle Stabilized Aqueous Foams at Different Length Scales: Synergy between Silica Particles and Alkylamines. Langmuir, 31(5), 1615–1622, 2015. [doi:10.1021/la503321m]
Carl, A.; Witte, J.; von Klitzing, R. A look inside particle stabilized foams-particle structure and dynamics. J. Phys. D: Appl. Phys., 48, 434003, 2015. [doi:10.1088/0022-3727/48/43/434003]
Fameau, A.-L.; Carl, A.; Saint-Jalmes, A.; von Klitzing, R. Responsive Aqueous Foams. ChemPhysChem, 16, 66-75, 2015. [doi:10.1002/cphc.201402580]
Paul, N.; Kraume, M.; Schön, S.; von Klitzing, R. Transport processes at single droplets in micellar liquid/liquid systems. AIChE J., 61(3), 1092–1104, 2015. [doi: 10.1002/aic.14699]
Carl, F. A. Stabilization of foams by in-situ hydrophobized nanoparticles. Technische Universität Berlin, 2016. [More]