Surface interaction and dynamics of molecular spin-probes as guests in tailor-made organosilica, porous hosts for applications in chromatography.
Solid State and Surface Chemistry, Material Synthesis
Final Report Abstract
Mass transport in, trough and out of porous solids is a deciding factor in a number of applications in process engineering, e.g. chromatography. One has to consider a hierarchical process, spanning several orders of length- and time-scales. At the molecular scale, in the range of few nanometers and picoseconds, there is a complex interplay between guest-solvent and guest-surface interactions, and this determines directly the mobility of those guests inside the porous materials. A comprehensive and scale-spanning, experimentally underpinned understanding of the transport of dissolved molecular species inside (functionalized) porous matrices is pivotal for realizing porous solids designated for particular applications (e.g. chromatography) by design rather than by empiricism. However, it is very difficult to "spot" the confined guests with sufficient temporal and spatial resolution at technically relevant conditions (in the presence of solvents and at T ≥ r.t.). We have successfully established electron spin resonance (ESR) spectroscopy as an analytical "eye". We have advanced the ESR methodology, aiming at more precise and first and foremost scale-spanning insights into the diffusion of molecular spin probes in pores. Furthermore, we have established a direct link between the synthesis of tailor-made, porous materials, which will enable to exert a much more controlled influence on the mass transport of dissolved species. We have also applied imaging ESR spectroscopy. The imaging methodology allows recording the spectroscopic signature of the guests at every position of the porous material. From these data we obtained information about the local dynamics and mobility, and at the same time we have analysed the mass transport through the porous medium at macroscopic dimensions. The direct correlation between molecular and macroscopic transport will in the future enable to investigate the separation of a compound mixture, by means of spectroscopy using two different spin probes and also for the concrete application, a chromatographic measurement.
Publications
- Journal of Physical Chemistry C 2013, 117, 2805
M. Wessig, M. Drescher, S. Polarz
(See online at https://doi.org/10.1021/jp310226f) - Angewandte Chemie-International Edition 2015, 54, 10465
A. Schachtschneider, M. Wessig, M. Spitzbarth, A. Donner, C. Fischer, M. Drescher, S. Polarz
(See online at https://doi.org/10.1002/anie.201502878) - Journal of Physical Chemistry C 2015, 119, 17474
M. Spitzbarth, M. Wessig, T. Lemke, A. Schachtschneider, S. Polarz, M. Drescher
(See online at https://doi.org/10.1021/acs.jpcc.5b05743) - Physical Chemistry Chemical Physics 2015, 17, 15976
M. Wessig, M. Spitzbarth, M. Drescher, R. Winter, S. Polarz
(See online at https://doi.org/10.1039/c5cp01369k) - Journal of Magnetic Resonance 2017, 283, 45
M. Spitzbarth, A. Scherer, A. Schachtschneider, P. Imming, S. Polarz, M. Drescher
(See online at https://doi.org/10.1016/j.jmr.2017.08.008) - Langmuir 2017, 33, 11968
M. Wessig, M. Spitzbarth, A. Klaiber, M. Drescher, S. Polarz
(See online at https://doi.org/10.1021/acs.langmuir.7b02713) - University of Konstanz, 2017
Martin Wessig
- Journal of Physical Chemistry C 2018, 122, 5376
A. Pivtsov, M. Wessig, V. Klovak, S. Polarz, M. Drescher
(See online at https://doi.org/10.1021/acs.jpcc.7b10758)
