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Effect of sodium loading on Pt/ZrO2 during ethanol steam reforming

机译:钠加载对乙醇蒸汽重整过程中Pt / ZrO2的影响

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摘要

Ethanol steam reforming (ESR) was investigated on unpromoted and several sodium promoted Pt/ZrO2 catalysts. From DRIFTS experiments, the following steps during ESR were inferred: dissociation of ethanol to produce ethoxy species; oxidative dehydrogenation of ethoxy species to acetate; and acetate decomposition. Acetate decomposition depends on the catalyst formulation. Decarboxylation is the most favored route at high sodium loading (2.5 and 5 wt.%); acetate decomposes in the forward direction to CH4 and a carbonate, which further decomposes to CO2. In contrast, decarbonylation is prevalent for the unpromoted catalyst or catalysts having low sodium loading. Acetate likely decomposes to CH3OH and CO. Adsorbed methanol may undergo further steam reforming by oxidative dehydrogenation to formate species, which decarbonylates via reverse decomposition to CO and H2O. Temperature programmed desorption/reaction and activity data confirmed that alkali promotion, especially at 1.8 %Na and higher loading, facilitates the forward acetate decomposition step, favoring decarboxylation over decarbonylation.
机译:研究了乙醇水蒸气重整(ESR)在未经修饰和几种钠促进的Pt/ZrO2催化剂上的反应。根据DRIFTS实验,推断ESR过程中的以下步骤:乙醇离解生成乙氧基物种;乙氧基物种氧化脱氢为醋酸盐;醋酸分解。醋酸盐分解取决于催化剂配方。脱羧是高钠负荷(2.5和5 wt.%)时最有利的途径;醋酸盐向前分解为CH4和碳酸盐,后者进一步分解为CO2。相比之下,脱羰反应普遍适用于未经修饰的催化剂或钠含量较低的催化剂。醋酸盐可能分解为CH3OH和CO。吸附的甲醇可能通过氧化脱氢进一步进行蒸汽重整,生成甲酸盐,甲酸盐通过反向分解为CO和H2O脱羰基。程序升温脱附/反应和活性数据证实,碱促进,尤其是在1.8%Na和更高负载下,有利于向前的醋酸盐分解步骤,有利于脱羧而非脱羰基。

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