Auto-Thermal Reforming Catalysts for Use in Chemical Looping Systems

DOE Phase I Contract No. DE-FG02-04ER83936

Steam reforming of methane is the current process for converting methane into synthesis gas. This is a very energy intensive process. Technology developed in this program was aimed at providing a novel, more economical and environmentally friendly way of spontaneously converting methane to synthesis gas for the subsequent production of hydrogen, liquid fuels, and commodity chemicals.

This project addressed the development of metal oxide catalysts for the chemical looping partial oxidation of natural gas to promote the production of synthesis gas. The catalysts developed here possessed the following attributes: high methane conversion and CO selectivity, long term stability, and reasonable cost. The catalysts were created for use in a chemical looping system which itself would help reduce capital and processing costs, reduce emissions of CO2 and nitrogen oxides, while allowing for easier separation of products.

A number of metal oxide and supported metal oxide catalysts were identified in Phase I which were shown capable of utilizing stored oxygen to promote the partial oxidation (POM) of a pure stream of methane during the catalyst reduction cycle. These catalysts also showed little or no decline in activity towards the subject chemistry over 10–15 redox cycles, proved resistant to or, in some cases, were aided by sulfur impurities; showed no negative affects from steam addition (up to 12%); and demonstrated CO/(CO+CO2) selectivities over 93% and methane conversion of >90% in some cases.

The increasing demand for hydrogen, push towards a hydrogen economy, stricter air quality standards, and ever increasing demand to end dependence on foreign oil renders these catalysts and chemical looping technology attractive. The catalysts developed here and the overall process would provide an avenue for hydrogen and syngas production for commodity chemicals which would rely on natural gas, and other methane sources, rather than foreign oil, would have minimal CO2 and nitrogen oxide emissions, and could easily be integrated into a system for hydrogen production including.