Project Details
Projekt
Control of the formation and reaction of copper-oxygen adduct complexes in multiphase streams
Applicant
Professorin Dr. Sonja Herres-Pawlis
Subject Area
Inorganic Molecular Chemistry - Synthesis and Characterisation
Chemical and Thermal Process Engineering
Chemical and Thermal Process Engineering
Term
from 2014 to 2022
Project identifier
Deutsche Forschungsgemeinschaft (DFG) - Project number 256729061
Within the SPP1740, the task of the Herres-Pawlis group was the development of tailored chemical reaction systems. The investigations targeted systems which react with oxygen and nitrogen monoxide for a detailed understanding of the processes in multiphase mixtures, as are present in reactive bubbly flows. Most important requirement is the tunable reaction speed as well as the sensitivity towards different measurement methods in order to probe in space- and time-resolved manner the reaction with the gas. Here, in situ spectroscopic methods are in the focus, e.g. Raman and fluorescence spectroscopy. Six different reaction systems have been developed and investigated towards their kinetic and theoretical aspects by means of stopped-flow spectroscopy, in the super focus mixer and in the Taylor bubble.The goal of the second funding period is to detect multidimensionally the oxygen transfer with subsequent consecutive or parallel reaction with mixing sensitivity and to elucidate the complete kinetics with mass transfer coefficients. Herefore, the system shall be detectable by LIF and be available in large quantities. The special challenge lies in tuning of the systems to room temperature whereby the defined Cu2O2 chemistry normally proceeds at -80°C. This is only possible by sophisticated ligand design. Additionally, strategies for the ligand recycling have to be developed in order to cover the required amounts within the SPP1740. The characterisation of the kinetics of oxygen activation and transfer will be performed by UV/Vis and stopped-flow spectroscopy in order to obtain the intrinsic reaction constants. In collaboration with selected working groups, multidimensional experiments in the super focus mixer, the Taylor-bubble, Taylor-flow, one- and two bubble cells, helical capillary flow reactors up to the bubble column are envisioned: herefore the colour of the generated systems but also their fluorescence response is utilised. A comprehensive kinetic analysis of all steps as well as a deep understanding of the mass transfer through the phase boundary layer gas-liquid is needed for the usage of the oxygenation reactions in technical scale. Here, simulation will aid in all size scales: density functional theory will help to model the atomistic steps of the most promising systems whereas further SPP partners simulate the kinetics in the super focus mixer, the Taylor bubble and the capillary flow reactor. Compared to the first project phase competitive-parallel and consekutive reactions will be studied.
DFG Programme
Priority Programmes
