Ring-Expansion Metathesis Polymerization Under Confinement
P. Probst, M. Lindemann, J. R. Bruckner, B. Atwi, D. Wang, F. R. Fischer, M. Högler, M. Bauer, N. Hansen, M. Dyballa and M. R. Buchmeiser J. Am. Chem. Soc. 2025, 147, 8741–8750.
Project C05
Simulation of diffusion-reaction processes
A hierarchical modelling framework to simulate diffusion-reaction processes in mesoporous confinement
A multiscale approach linking simulation data obtained in model pores at atomistic resolution with realistic geometrical models of mesopore space based on physical reconstruction is developed with the aim to deconvolute, understand, predict and utilize confinement effects in molecular heterogeneous catalysis. Close feedback to continuous flow experiments and advanced diffraction analysis will provide an unprecedented high-resolution picture of the confined reaction space on the one hand and numerical models, capable to describe macroscopic behavior, on the other.
Research Questions
- How do pore diameter and pore surface influence diffusion and density profiles of solvent, reactants and products?
- How does pore geometry affect mass transport and molecular distribution?
- Can the solvent be tuned to optimize catalytical reactivity and selectivity?
- What are the most essential parameters in a multiscale modelling approach?
Influence of Ionic Liquid Film Thickness and Flow Rate on Macrocyclization Efficiency and Selectivity in Supported Ionic Liquid-Liquid Phase Catalysis
M. Högler, T. Kobayashi, H. Kraus, B. Atwi, M. R. Buchmeiser, M. Fyta and N. Hansen Chem. Eur. J. 2025, 31, e202403237.
Effects of Surfaces and Confinement on Formic Acid Dehydrogenation Catalyzed by an Immobilized Ru–H Complex: Insights from Molecular Simulation and Neutron Scattering
H.-H. Nguyen, M. Högler, N. Schnabel, N. Hansen, T. Sottmann and D. P. Estes ACS Catal. 2024, 14, 11252–11261.
Probing Self-Diffusion of Guest Molecules in a Covalent Organic Framework: Simulation and Experiment
L. Grunenberg, Ch. Keßler, T. Wei Teh, R. Schuldt, F. Heck, J. Kästner, J. Groß, N. Hansen and B. V. Lotsch ACS Nano 2024, 18, 25, 16091–16100.
Axial Diffusion in Liquid-Saturated Cylindrical Silica Pore Models
H. Kraus, M. Högler and N. Hansen J. Phys. Chem. C 2023, 127, 29, 14374–14388.
Influence of layer slipping on adsorption of light gases in covalent organic frameworks: A combined experimental and computational study
C. Kessler, R. Schuldt, S. Emmerling, B. Lotsch, J. Kästner, J. Groß and N. Hansen
Microporous Mesoporous Mater. 2022, 336, 111796.
An atomistic view on the uptake of aromatic compounds by cyclodextrin immobilized on mesoporous silica
H. Kraus and N. Hansen
Adsorption 2022, 28, 125–136.
Confinement Effects for Efficient Macrocyclization Reactions with Supported Cationic Molybdenum Imido Alkylidene N‑Heterocyclic Carbene Complexes
F. Ziegler, H. Kraus, M. J. Benedikter, D. Wang, J. R. Bruckner, M. Nowakowski, K. Weißer, H. Solodenko, G. Schmitz, M. Bauer, N. Hansen and M. R. Buchmeiser ACS Catal. 2021, 11, 11570-11578.
Adsorption of light gases in covalent organic frameworks: comparison of classical density functional theory and grand canonical Monte Carlo simulations
C. Kessler, J. Eller, J. Groß and N. Hansen Microporous Mesoporous Mater. 2021, 111263.
PoreMS: a software tool for generating silica pore models with user-defined surface functionalisation and pore dimensions
H. Kraus, J. Rybka, A. Höltzel, N. Trebel, U. Tallarek and N. Hansen Mol. Simul. 2021, 47, 306-316.
Confined Ru‐catalysts in a Two‐phase Heptane/Ionic Liquid Solution: Modeling Aspects
T. Kobayashi, H. Kraus, N. Hansen and M. Fyta ChemCatChem 2021, 13, 739– 746.
Olefin Metathesis in Confined Geometries: A Biomimetic Approach toward Selective Macrocyclization
F. Ziegler, J. Teske, I. Elser, M. Dyballa, W. Frey, H. Kraus, N. Hansen, J. Rybka, U. Tallarek and M.R. Buchmeiser J. Am. Chem. Soc. 2019, 141, 19014-19022.
Rotational barriers of carbamate-protected amine crosslinkers for hydrogels: A combined experimental and computational study
N. Schädel, J. Gebhardt, M. Löffler, D. Garnier, N. Hansen and S. Laschat J. Phys. Org. Chem. 2019, 32, e3936.