Christian WICK1, David SMITH2, Ana-Sun?ana SMITH1
1Friedrich-Alexander-Universität Erlangen-Nürnberg, PULS Group and Competence Unit for Scientific Computing, Erlangen, Germany
2Ru?er Bokovi? Institute, Zagreb, Croatia
We present a sequential multiscale modelling approach to investigate the influence of the molecular environment on the chemical reactions and structuring in Supported ionic liquid phase (SILP) catalysts. SILP are designer catalysts comprising molecular (transition metal) catalytic compounds dissolved in an ionic liquid (IL) thin film covering a porous support. The choice of molecular catalyst dissolved in the IL controls the envisaged chemical reactions, while the reaction conditions can be controlled and fine-tuned via variation of the support, the IL and, furthermore, by addition of organic or inorganic additives. Using taskspecific IL / catalyst combinations and two different types of chemical reactions (Water-Gas-Shift and hydrogenation), we elucidate the effects of the SILP composition on the chemical reactivity by density functional and ab initio calculations, which are corroborated by (in situ) experiments. Additives can either function as small molecule shuttles [1,2] or directly influence the reaction mechanism [3,4] by non-covalent effects. While the effect of the environment in the IL phase is already clearly visible at a continuum description, we aim at a more detailed understanding of the structuring and interface enrichments at the molecular scale by means of classical molecular dynamics simulations, which were validated against experiments [5,6]. Ultimately, we aim at combining our experience from our sequential-multiscale modelling to conduct hybrid QM/MM calculations directly incorporating the effects of the molecular environment on the chemical reactivity in SILP catalysts.
 P. Wolf, M. Aubermann, M. Wolf, T. Bauer, D. Blaumeiser, R. Stepic, C. R. Wick, D. M. Smith, A.-S. Smith, P. Wasserscheid, J. Libuda, M. Haumann, Green Chem. 21 (2019) 5008–5018.
 D. Blaumeiser, R. Stepi?, P. Wolf, C. R. Wick, M. Haumann, P. Wasserscheid, D. M. Smith, A.-S. Smith, T. Bauer, J. Libuda, Catal. Sci. Technol. 10 (2020) 252–262.
 P. Wolf, C.R. Wick, J. Mehler, D. Blaumeiser, S. Schötz, T. Bauer, J. Libuda, D. Smith, A.-S. Smith, M. Haumann, ACS Catal (2022) 12.
 R. Stepi?, C.R. Wick, V. Strobel, D. Berger, N. Vu?emilovi??Alagi?, M. Haumann, P. Wasserscheid, A.-S. Smith, D.M. Smith, Angew. Chem. Int. Ed. 58 (2019) 741–745.
 V. Seidl, M. Bosch, U. Paap, M. Livraghi, Z. Zhai, C.R. Wick, T.M. Koller, P. Wasserscheid, F. Maier, A.-S. Smith, J. Bachmann, H.-P. Steinrück, K. Meyer, J. Ion. Liq. 2 (2022) 100041.
 N. Vu?emilovi?-Alagi?, R.D. Banhatti, R. Stepi?, C.R. Wick, D. Berger, M.U. Gaimann, A. Baer, J. Harting, D.M. Smith, A.-S. Smith, J. Colloid Interface Sci. 553 (2019) 350–363.