2019
DOI: 10.1021/acs.iecr.9b01267
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The Effect of Prereduction on the Performance of Pd/Al2O3 and Pd/CeO2 Catalysts during Methane Oxidation

Abstract: Pd/Al2O3 and Pd/CeO2 catalysts were investigated for methane oxidation at conditions typical for the exhaust of lean burn gas engines. The results show that catalyst prereduction significantly increases the catalytic activity during the light-off irrespective of the gas composition. Operando X-ray absorption spectroscopy revealed a fully reduced catalyst state after the reductive pretreatment, which is reoxidized with increasing temperature in a lean reaction mixture, resulting in bulk PdO formation at 350 °C.… Show more

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Cited by 67 publications
(74 citation statements)
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“…This procedure can be referred to as "catalyst degreening" and is common when studying supported noble metal catalysts. 53,54 The corresponding final extinction profiles for the remaining catalysts are included in Fig. S3.…”
Section: Methane Oxidation Kineticsmentioning
confidence: 99%
“…This procedure can be referred to as "catalyst degreening" and is common when studying supported noble metal catalysts. 53,54 The corresponding final extinction profiles for the remaining catalysts are included in Fig. S3.…”
Section: Methane Oxidation Kineticsmentioning
confidence: 99%
“…Figure 5 shows an expected trend of Pd(0) decrease with the temperature increase, and the metal oxidation rate is suppressed by the presence of water. [7,9,10] However, the SnO 2 /SnO support promotes the formation of PdO, while mostly Pd(OH) 2 is observed on the Al 2 O 3 support. To evaluate the metal oxide interaction with water, we calculated standard Gibbs free energies of endothermic dehydroxylation reactions R(1)-R(3) [Eqs.…”
Section: In Situ Xas: Sn L 3 Edge During Wet Methane Combustionmentioning
confidence: 99%
“…[3] Our earlier in situ X-ray absorption spectroscopy study provided evidence of the lack of oxygen at Pd active sites in the wet feed at low temperatures in Pd/Al 2 O 3 system, [9] which was supported by others. [10] Among a myriad of reported catalysts, SnO 2 -supported Ptgroup materials have a rather extraordinary resistance to water poisoning in wet methane combustion. [11,12] We have previously shown ( Figure 1 [13] ) that Pd/SnO 2 can surpass even PdÀ Pt/Al 2 O 3 in its activity in the presence of water; studies by others [11] and ourselves [13] also report insignificant variations in methane conversion when the water content in the feed was increased up to 20 %.…”
Section: Introductionmentioning
confidence: 99%
“…Amongst these properties, the catalyst is moreover influenced by the support material [18,19] and by further noble metal dopants such as platinum [20,21]. Furthermore, Lott et al recently described an enhanced oxidation performance for pre-reduced PdO catalysts in the presence and absence of externally dosed water, pointing to a strong dependence of the catalytic activity on the catalyst history [22,23]. All the mentioned aspects result in the complex non-linear behavior of the catalytic PdO system.…”
Section: Introductionmentioning
confidence: 99%