A chemical looping process using the redox reactions of iron oxide has been used to produce separate streams of pure H-2 and CO2 from a solid fuel. An iron oxide carrier prepared using a mechanical mixing technique and comprised of 100 wt.% Fe2O3 was used. It was demonstrated that hydrogen can be produced from three representative coals - a Russian bituminous, a German lignite and a UK sub-bituminous coal. Depending on the fuel, pure H-2 with [CO] less than or similar to 50 vol. ppm can be obtained from the proposed process. The cyclic stability of the iron oxide carrier was not adversely affected by contaminants found in syngas which are gaseous above 273 K. Stable quantities of H-2 were produced over five cycles for all three coals investigated. Independent of the fuel, SO2 was not formed during the oxidation with steam, i.e. the produced H-2 was not contaminated with SO2. Since oxidation with air removes contaminants and generates useful heat and pure N-2 for purging, it should be included in the operating cycle. Overall, it was demonstrated that the proposed process may be an attractive approach to upgrade crude syngas produced by the gasification of low-rank coals to pure H-2, representing a substantial increase in calorific value, whilst simultaneous capturing CO2, a greenhouse gas. (C) 2010 Elsevier B.V. All rights reserved.