CO2 Splitting in a Hot-Wall Aerosol Reactor via the Two-Step Zn/ZnO Solar Thermochemical Cycle

Abstract

Using concentrated solar energy as the source of high-temperature process heat, a two-step CO2 splitting thermochemical cycle based on Zn/ZnO redox reactions is applied to produce renewable carbon-neutral fuels. The solar thermochemical cycle consists of: 1) the solar endothermic dissociation of ZnO to Zn and O2; 2) the non-solar exothermic reduction of CO2 with Zn to CO and ZnO; the latter is the recycled to the 1st solar step. The net reaction is CO2 = CO + 1/2 O2, with products formed in different steps, thereby eliminating the need for their separation. A Second-Law thermodynamic analysis indicates a maximum solar-to-chemical energy conversion efficiency of 39% for a solar concentration ratio of 5000 suns. The technical feasibility of the first step of the cycle has been demonstrated in a high-flux solar furnace with a 10 kW solar reactor prototype. The second step of the cycle is experimentally investigated in a hot-wall quartz aerosol flow reactor, designed for in-situ quenching of Zn(g), formation of Zn nanoparticles, and oxidation with CO2. The effect of varying the molar flow ratios of the reactants was investigated. Chemical conversions were determined by gas chromatography and X-ray diffraction. Chemical conversions of Zn to ZnO of up to 88% were obtained for a residence time of ∼ 3.05 s. For all of the experiments, the reactions primarily occurred outside the aerosol jet flow on the surfaces of the reaction zone.