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Lattice Oxygen and Feed Oxygen Exchange for the High Rate of H.sub.2 + O.sub.2 Recombination on Ti.sub.1-xPd.sub.xO.sub.2-x Catalyst at Room Temperature
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Lattice Oxygen and Feed Oxygen Exchange for the High Rate of H.sub.2 + O.sub.2 Recombination on Ti.sub.1-xPd.sub.xO.sub.2-x Catalyst at Room Temperature
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Lattice Oxygen and Feed Oxygen Exchange for the High Rate of H.sub.2 + O.sub.2 Recombination on Ti.sub.1-xPd.sub.xO.sub.2-x Catalyst at Room Temperature
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Journal Article
Lattice Oxygen and Feed Oxygen Exchange for the High Rate of H.sub.2 + O.sub.2 Recombination on Ti.sub.1-xPd.sub.xO.sub.2-x Catalyst at Room Temperature
2024
Overview
The Pd ion substituted TiO.sub.2, synthesized by solution combustion method crystallizes in anatase structure with stable composition Ti.sub.1-xPd.sub.xO.sub.2-x (x = 0.01-0.03) creating an oxide ion vacancy per Pd.sup.2+ ion substitution. Over 1.35 mol of H.sub.2 per mole of bulk Pd ions, in 5 nm nanocrystalline catalyst Ti.sub.1-xPd.sub.xO.sub.2-x (x = 0.03) is adsorbed at 300 K. On exposure of only hydrogen to Ti.sub.0.98Pd.sub.0.02O.sub.1.98 at 300 K, water is formed making the catalyst wet. On heating in a vacuum, mass loss due to water is 0.026 mol /mole of catalyst meaning 1.3 mol of hydrogen per mole of Pd ion in the catalyst. Pd ion substitution in TiO.sub.2 anatase activates lattice oxygen leading to the formation of H.sub.2O on exposure to H.sub.2 gas at 300 K utilizing lattice oxygen. On heating in air at 650 K the reduced catalyst is regenerated. The catalyst produces a high rate of H.sub.2 + O.sub.2 recombination up to 9 [micro]moles.sup.-1 g.sup.-1 at 300 K, and over 230 [micro]moles.sup.-1 g.sup.-1 at 330 K with a TOF of 2000 h.sup.-1. The catalyst is coated on cordierite honeycomb avoiding handling of powder catalyst. The rates are highest compared to any catalyst for H.sub.2 + O.sub.2 recombination known so far. Extensive DFT calculation on (101) surface in Ti.sub.31Pd.sub.1O.sub.63 slab confirmed (a) one oxygen out of 4 bonded to Pd ion in nearly square geometry is fully activated to form water molecule creating an oxide ion vacancy; (b) dissociative adsorption of H.sub.2 on one of the Pd as well as oxide ion and not both on Pd ion; (c) exchange of feed oxygen with lattice oxygen during 2H.sub.2 + O.sub.2 recombination; (d) 2H.sub.2 + O.sub.2 [right arrow] 2H.sub.2O molecules form per Pd ion in one cycle regenerating the catalyst, Ti.sub.0.97Pd.sub.0.03O.sub.1.97 surface explaining high rates of recombination and (e) Pd ion undergoes redox cycle with Ti and oxide ions acting as charge reservoirs.
Publisher
Springer
Subject
