Rapid solar-thermal decarbonization of methane

Due to the ever-increasing demand for energy and the concern over the environmental impact of continuing to produce energy using current methods, there is interest in developing a hydrogen economy. Hydrogen is a desirable energy source because it is abundant in nature and burns cleanly. One method for producing hydrogen is to utilize a renewable energy source to obtain high enough temperatures to decompose a fossil fuel into its elements. This thesis work is directed at developing a solar-thermal aerosol flow reactor to dissociate methane to carbon black and hydrogen. The technology is intended as a “bridge” between current hydrogen production methods, such as conventional steam-methane reformers, and future “zero emission” technology for producing hydrogen, such as dissociating water using a renewable heating source. A solar furnace is used to heat a reactor to temperatures in excess of 2000 K. The final reactor design studied consists of three concentric vertical tubes—an outer quartz protection tube, a middle solid graphite heating tube, and an inner porous graphite reaction tube. A “fluid-wall” is created on the inside wall of the porous reaction tube in order to prevent deposition of the carbon black co-product on the reactor tube wall. The amorphous carbon black produced aids in heating the gas stream by absorbing radiation from the reactor wall. Conversions of 90% are obtained at a reactor wall temperature of 2100 K and an average residence time of 0.01 s. Computer modeling is also performed to study the gas flow and temperature profiles in the reactor as well as the kinetics of the methane dissociation reaction. The simulations indicate that there is little flow of the fluid-wall gas through the porous wall in the hot zone region, but this can be remedied by increasing the inlet temperature of the fluid-wall gas and/or increasing the tube permeability only in the hot zone region of the wall. The following expression describes the kinetics of methane dissociation in a solar-thermal fluid-wall reactor: dXdt=5.8×10⁸ exp-155,600RT 1-X ^7.2s^-1. The experimental and theoretical work reported in this thesis is the groundwork that will be utilized in scaling up the reactor to produce hydrogen in distributed or centralized facilities.