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Computational Analytical Chemistry: Molecular-Level Understanding of Interfacial Phenomena including Reversed Phase Liquid Chromatography from Atomistic Simulations

Applicant Meuwly Markus
Number 134954
Funding scheme Project funding
Research institution Physikalische Chemie Departement Chemie Universität Basel
Institution of higher education University of Basel - BS
Main discipline Physical Chemistry
Start/End 01.04.2011 - 28.02.2014
Approved amount 154'138.00
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Keywords (4)

Molecular Dynamics; Water Filaments; Chemical Interfaces; Infrared Spectroscopy

Lay Summary (English)

Lead
Lay summary
The goal of this project is to understand the role of solvent
molecules at interface, in particular those relevant to reversed phase
liquid chromatography (RPLC). RPLC is one of the most powerful methods
for separating a mixture of compounds but the atomistic processes
underlying it are still poorly understood. One of the reasons is that
structural data is difficult to obtain because the systems are
disordered (amorphous) and conventional structure-sensitive methods
such as X-Ray spectroscopy are inappropriate. Two techniques have been
successfully applied in the past to still obtain atom-level
understanding: atomistic simulations and surface-sensitive
spectroscopy. In this project we use atomistic simulations to
investigate the dynamics of the solvent (water and small
surface-active compounds including acetonitrile and methanol) at the
interface which consists of a functionalized silica surface. In
parallel, we also try to make contact with the spectroscopic data
through explicit simulation of the infrared spectra which in turn can
be translated into structural information which is possible because
from a simulation both, position and velocity of the atoms are known.
Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Dynamics and vibrational spectroscopy of water at hydroxylated silica surfaces.
Gupta Prashant Kumar, Meuwly Markus (2013), Dynamics and vibrational spectroscopy of water at hydroxylated silica surfaces., in Faraday discussions, 167, 329-46.
Dynamics of Water/Methanol Mixtures at Functionalized Chromatographic Interfaces
Gupta PK, Meuwly M (2012), Dynamics of Water/Methanol Mixtures at Functionalized Chromatographic Interfaces, in JOURNAL OF PHYSICAL CHEMISTRY B, 116(35), 10951-10959.
Structure, spectroscopy and dynamics of layered H(2)O and CO(2) ices.
Lee Myung Won, Plattner Nuria, Meuwly Markus (2012), Structure, spectroscopy and dynamics of layered H(2)O and CO(2) ices., in Physical chemistry chemical physics : PCCP, 14(44), 15464-74.
Diffusion of Atomic Oxygen Relevant to Water Formation in Amorphous Interstellar Ices
Myung Won Lee and Markus Meuwly, Diffusion of Atomic Oxygen Relevant to Water Formation in Amorphous Interstellar Ices, in Faraday Discussions.

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
Faraday Discussion 168 Talk given at a conference Oxygen Migration in Amorphous Ices 07.04.2014 Leiden, Netherlands Meuwly Markus;
Faraday Discussion 167 Talk given at a conference Dynamics and Spectroscopy at Silca Surfaces 17.09.2013 Bristol, Great Britain and Northern Ireland Meuwly Markus; Gupta Prashant Kumar;
NCCR MUST Annual Meeting Talk given at a conference Computer Simulations of Condensed Phase Phenomena 07.01.2013 Engelberg, Switzerland Gupta Prashant Kumar; Meuwly Markus;
Theoretical Chemistry Symposium 2012 Talk given at a conference Computational Chromatography 19.12.2012 IIT Guwahati, India Gupta Prashant Kumar;
Fall Meeting Swiss Chemical Society 2012 Poster Computational Chromatography 13.09.2012 ETH Zurich, Switzerland Gupta Prashant Kumar; Meuwly Markus;
Hands-On' Workshop on Computational Biophysics at Bremen Poster Computational Chromatography 17.10.2011 Bremen / DE, Germany Gupta Prashant Kumar;
25th Molecular Modelling Workshop 2011 Talk given at a conference Multipolar force fields for simulations 04.04.2011 Erlangen / DE, Germany Meuwly Markus; Gupta Prashant Kumar;


Associated projects

Number Title Start Funding scheme
121806 Computational Analytical Chemistry: Atomistic and Coarse Grained Simulations of Reversed Phase Liquid Chromatography 01.03.2009 Project funding

Abstract

The goal of the project is to develop and apply quantitative numericalmethods and computational strategies to understand thephysico-chemical properties of interfacial systems, in particularrelevant to reversed phase liquid chromatography (RPLC). RPLC is awidely used analytical technique in pharmaceutical separations, thefood industry, in life-science applications (peptide and proteinseparation), and in the analysis of industrial polymers. Despite thisimportance (up to 90 \% of all analytical separations on low molecularweight samples use RPLC) the molecular mechanisms for retention andselectivity are still unclear. Important questions that we addresshere include the potentially active role played by the solvent and itscomposition, the influence of the (chemical) functionalization on thedynamics of the solvent and solute at the interface, and themorphology of the solid and mobile phase at the interface. Vibrationalspectroscopy has emerged as one of the prime techniques tocharacterize the solvent (in particular water) at the solid/liquidinterface. Using and further developing multipolar force fields,structural aspects of water and solvent organization at the interfacewill be addressed. Finally, the dynamics of probe molecules (includingacridine orange, naphthalene, butylbenzene, 2-nitrobenzoic acid,coumarin and other polycyclic aromatic hydrocarbons) for whichexperimental data is available will be investigated. Such questionsare ideally suited to be pursued with computer simulations which arealso validated in view of experimental data.
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