Design and Characterization of a Novel Upward Flow Reactor for the Study of High-Temperature Thermal Reduction for Solar-Driven Processes

Abstract

The design and characterization of an upward flow reactor (UFR) coupled to a high flux solar simulator (HFSS) under vacuum is presented. The UFR was designed to rapidly heat solid samples with concentrated irradiation to temperatures greater than 1000 °C at heating rates in excess of 50 K/s. Such conditions are ideal for examining high-temperature thermal reduction kinetics of reduction/oxidation-active materials by temporally monitoring O2 evolution. A steady-state, computational fluid dynamics (CFD) model was employed in the design to minimize the formation of eddies and recirculation, and lag and dispersion were characterized through a suite of O2 tracer experiments using deconvolution and the continuously stirred tank reactors (CSTR) in series models. A transient, CFD and heat transfer model of the UFR was combined with Monte Carlo ray tracing (MCRT) to determine radiative heat fluxes on the sample from the HFSS to model spatial and temporal sample temperatures. The modeled temperatures were compared with those measured within the sample during an experiment in which Co3O4 was thermally reduced to CoO and O2. The measured temperatures within the bed were bounded by the average top and bottom modeled bed temperatures for the duration of the experiment. Small variances in the shape of the modeled versus experimental temperatures were due to contact resistance between the thermocouple and particles in the bed and changes in the spectral absorptivity and emissivity as the Co3O4 was reduced to CoO and O2.