Transition from batch to continuous operation: Development and investigation of a process for the production of higher alcohols

  • Übertragung vom chargenweisen in den kontinuierlichen Betrieb: Entwicklung und Untersuchung eines Prozesses zur Darstellung höherer Alkohole

Schnoor, Johann-Kilian; Liauw, Marcel A. (Thesis advisor); Büchs, Jochen (Thesis advisor)

Aachen : RWTH Aachen University (2020, 2021)
Dissertation / PhD Thesis

Dissertation, RWTH Aachen University, 2020


This doctoral thesis is the result of research conducted as part of the Carbon2Chem project. The projects aim is the utilization of steel mill flue gases for the production of valuable chemicals, in particular higher alcohols. Currently neither a continuous homogeneously catalyzed reaction for the production of higher alcohols on an industrial scale from steel mill flue gases nor a protocol for the transition of batch reactions into continuous operation is available on a lab scale. This thesis aims to present a protocol and guideline for the transition of lab scale batch reactions into continuous operation. This protocol shall then be applied for the development of a multistage reaction for the production of higher alcohols from steel mill flue gases. For the successful process fluid dynamic phenomena are investigated and new inline and on-line analytic is developed, integrated, calibrated under process conditions and validated to allow real-time analysis for kinetic investigations of the reactions. As a result optimal process windows, reaction conditions and catalysts are identified for the different reactions. Organic solvent nanofiltration is identified as a very good method for catalyst recycling and product separation. The developed inline analysis based on infra-red spectroscopy has proven very versatile and allowed for quick and automated calibration and validation for different reaction mixtures leading to the determination of the reactions kinetics. The calibration under process conditions has proven as a very good method for using infra-red spectroscopy for different reagents in a continuous setup. The developed protocol for the transition into continuous operation has proven very successful in designing a versatile continuous reactor setup. A new method for the identification of process windows for spiral wound capillary reactors was developed. A new continuous process was developed by transferring a batch reaction for the production of higher alcohols into continuous operation. The reactions kinetics were determined to enable further modeling and scale-up of the process. Organic solvent nanofiltration was identified as a method for catalyst recycling and product separation of the reaction mixture in a single step.