Mixed metal oxides containing ceria and zirconia have been studied as high temperature desulfurization sorbents with the objective of achieving the DOE Vision 21 target of 1 ppmv or less H 2 S in the product gas. The research was justified by recent results in this laboratory that showed that reduced CeO 2 , designated CeO n (1.5 < n < 2.0), is capable of achieving the 1 ppmv target in highly reducing gas atmospheres. The addition of ZrO 2 has improved the performance of oxidation catalysts and three-way automotive catalysts containing CeO 2 , and was postulated to have similar beneficial effects on CeO 2 desulfurization sorbents.An electrochemical method for synthesizing CeO 2 -ZrO 2 mixtures was developed and the products were characterized by XRD and TEM during year 01. Nanocrystalline particles having a diameter of about 5 nm and containing from approximately 10 mol% to 80 mol% ZrO 2 were prepared. XRD analysis showed the product to be a solid solution at low ZrO 2 contents with a separate ZrO 2 phase emerging at higher ZrO 2 levels. Unfortunately, the quantity of CeO 2 -ZrO 2 that could be prepared electrochemically was too small to permit desulfurization testing.Also during year 01 a laboratory-scale fixed-bed reactor was constructed for desulfurization testing. All components of the reactor and analytical systems that were exposed to low concentrations of H 2 S were constructed of quartz, Teflon, or silcosteel. Reactor product gas composition as a function of time was determined using a Varian 3800 gas chromatograph equipped with a pulsed flame photometric detector (PFPD) for measuring low H 2 S concentrations from approximately 0.1 to 10 ppmv, and a thermal conductivity detector (TCD) for higher concentrations of H 2 S.Larger quantities of CeO 2 -ZrO 2 mixtures from other sources, including mixtures prepared in this laboratory using a coprecipitation procedure, were obtained. Much of the work during year 02 consisted of characterization and desulfurization testing of materials obtained from commercial sources. Most of the commercial CeO 2 and CeO 2 -ZrO 2 materials were capable of reducing H 2 S concentration from 5000 ppmv in highly reducing feed gas to less than 1 ppmv in the product gas. However, to properly evaluate the effect of ZrO 2 addition on desulfurization capability, the physical properties of the sorbent must be similar. That is, a CeO 2 -ZrO 2 mixture from source A would not necessarily be superior to pure CeO 2 from source B if the properties of the pure CeO 2 were superior. Therefore, research during year 03 concentrated on CeO 2 and CeO 2 -ZrO 2 mixtures prepared in this laboratory using a coprecipitation procedure. The structural properties of these sorbents were similar and the effect of ZrO 2 addition could better be separated from the structural effects.X-ray diffraction tests of the sorbents prepared in house confirmed the formation of a solid solution of ZrO 2 in CeO 2 . Crystallite sizes ranged from 12.7 to 18.8 nm and surface areas from 75 to 85 m 2 /g. Reduction tests us...