Integrated High Temperature Coal-to-Hydrogen System with CO2 Separation

A significant barrier to the commercialization of coal-to-hydrogen technologies is high capital cost. The purity requirements for H{sub 2} fuels are generally met by using a series of unit clean-up operations for residual CO removal, sulfur removal, CO{sub 2} removal and final gas polishing to achieve pure H{sub 2}. A substantial reduction in cost can be attained by reducing the number of process operations for H{sub 2} cleanup, and process efficiency can be increased by conducting syngas cleanup at higher temperatures. The objective of this program was to develop the scientific basis for a single high-temperature syngas-cleanup module to produce a pure stream of H{sub 2} from a coal-based system. The approach was to evaluate the feasibility of a 'one box' process that combines a shift reactor with a high-temperature CO{sub 2}-selective membrane to convert CO to CO{sub 2}, remove sulfur compounds, and remove CO{sub 2} in a simple, compact, fully integrated system. A system-level design was produced for a shift reactor that incorporates a high-temperature membrane. The membrane performance targets were determined. System level benefits were evaluated for a coal-to-hydrogen system that would incorporate membranes with properties that would meet the performance targets. The scientific basis for high temperature CO{sub 2}-selective membranes was evaluated by developing and validating a model for high temperature surface flow membranes. Synthesis approaches were pursued for producing membranes that integrated control of pore size with materials adsorption properties. Room temperature reverse-selectivity for CO{sub 2} was observed and performance at higher temperatures was evaluated. Implications for future membrane development are discussed