PMID- 21693898 OWN - NLM STAT- PubMed-not-MEDLINE DCOM- 20121002 LR - 20110622 IS - 0953-8984 (Print) IS - 0953-8984 (Linking) VI - 20 IP - 6 DP - 2008 Feb 13 TI - Design of water gas shift catalysts for hydrogen production in fuel processors. PG - 064237 LID - 10.1088/0953-8984/20/6/064237 [doi] AB - Low sulfur hydrocarbon fuels can be converted to fuel cell grade H(2) using a compact fuel processor architecture. The necessary high volumetric activity water gas shift (WGS) Pt on ceria-zirconia catalysts reacts CO-rich reformate with steam to yield H(2) and CO(2). Such highly selective, non-pyrophoric noble metal/Ce([1-(x+y)])Zr(x)Dp(y)O(2) catalysts were developed through coordinated atomic modeling, syntheses, structural characterization, kinetic performance tests, and micro-kinetic analyses. Density functional simulations made with the VASP code suggested that the undoped catalyst WGS activity would be limited by the strong binding of CO intermediates, blocking the reoxidation of the reduced oxide by water. These predictions were confirmed by in situ cylindrical internal reflection-Fourier transform infrared spectroscopy and by micro-kinetic analyses of the micro-reactor results. Atomic simulations were used to evaluate the impact transition metal dopants had on the surface chemistry of cubic ceria-zirconia. VASP predicted that acidic transition metal dopants such as Nb, Mo, Ta, and W would increase the oxide surface affinity for water and thus increase the turnover rate of the catalyst. The efficacy of Mo-doped ceria-zirconia compositions was confirmed at lower temperatures in replicated catalyst synthesis-reactor studies. FAU - Opalka, S M AU - Opalka SM AD - United Technologies Research Center, East Hartford, CT 06108, USA. FAU - Vanderspurt, T H AU - Vanderspurt TH FAU - Radhakrishnan, R AU - Radhakrishnan R FAU - She, Y AU - She Y FAU - Willigan, R R AU - Willigan RR LA - eng PT - Journal Article DEP - 20080124 PL - England TA - J Phys Condens Matter JT - Journal of physics. Condensed matter : an Institute of Physics journal JID - 101165248 EDAT- 2008/02/13 00:00 MHDA- 2008/02/13 00:01 CRDT- 2011/06/23 06:00 PHST- 2011/06/23 06:00 [entrez] PHST- 2008/02/13 00:00 [pubmed] PHST- 2008/02/13 00:01 [medline] AID - S0953-8984(08)58791-1 [pii] AID - 10.1088/0953-8984/20/6/064237 [doi] PST - ppublish SO - J Phys Condens Matter. 2008 Feb 13;20(6):064237. doi: 10.1088/0953-8984/20/6/064237. Epub 2008 Jan 24.