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CO adsorption and correlation between CO surface coverage and activity/selectivity of preferential CO oxidation over supported Ag catalyst: an in situ FTIR study

机译:CO adsorption and correlation between CO surface coverage and activity/selectivity of preferential CO oxidation over supported ag catalyst: an in situ FTIR study

摘要

In situ IR measurements for CO adsorption and preferential CO oxidation in H-2-rich gases over Ag/SiO2 catalysts are presented in this paper. CO adsorbed on the Ag/SiO2 pretreated with oxygen shows a band centered around 2169 cm(-1), which is assigned to CO linearly bonded to Ag+ sites. The amount of adsorbed CO on the silver particles ( manifested by an IR band at 2169 cm(-1)) depends strongly on the CO partial pressure and the temperature. The steady-state coverage on the Ag surface is shown to be significantly below saturation, and the oxidation of CO with surface oxygen species is probably via a non-competitive Langmuir Hinshelwood mechanism on the silver catalyst which occurs in the high-rate branch on a surface covered with CO below saturation. A low reactant concentration on the Ag surface indicates that the reaction order with respect to Pco is positive, and the selectivity towards CO2 decreases with the decrease of Pco. On the other hand, the decrease of the selectivity with the reaction temperature also reflects the higher apparent activation energy for H-2 oxidation than that for CO oxidation.
机译:本文介绍了在原位红外测量中,与Ag / SiO2催化剂相比,富H-2气体中的CO吸附和优先CO氧化。吸附在用氧气预处理的Ag / SiO2上的CO显示出一条以2169 cm(-1)为中心的谱带,该谱带分配给线性键合到Ag +位点上的CO。银颗粒上的CO吸附量(由2169 cm(-1)处的IR带显示)在很大程度上取决于CO分压和温度。已证明Ag表面的稳态覆盖率显着低于饱和,并且CO与表面氧的氧化可能是通过银催化剂上高速率分支中发生的非竞争性Langmuir Hinshelwood机制在银催化剂上发生的。饱和度以下的CO覆盖的表面。 Ag表面上的低反应物浓度表明相对于Pco的反应顺序为正,并且随着Pco的降低,对CO 2的选择性降低。另一方面,随着反应温度选择性的降低也反映出H-2氧化的表观活化能高于CO氧化的表观活化能。

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