负载钯催化剂上亚硝酸乙酯的催化分解

Catalytic Decomposition of Ethyl Nitrite over Supported Palladium Catalyst

研究了亚硝酸乙酯在不同载体及负载钯催化剂上的分解行为 .结果显示 ,固体酸性中心和金属钯中心都可以催化亚硝酸乙酯的分解反应 .在C2 H5ONO与CO合成草酸二乙酯的反应中 ,亚硝酸乙酯是在固体催化剂表面发生分解 ,而不是在气相发生热裂解 .并且 ,该反应的活性与亚硝酸乙酯的分解程度不存在正比关系 .通过对分解产物的分析 ,提出了亚硝酸乙酯在固体催化剂上分解的连续脱氢机理 .

The decomposition of ethyl nitrite over different supports and supported palladium catalysts was investigated. The results revealed that both the solid acid sites and the Pd active sites can catalyze this decomposition reaction. The main products contained ethanol, ethane diethoxy, acetaldehyde and ethyl acetate. For γ-Al 2O 3, the conversion of C 2H 5ONO was ca 30% at 120 ℃, while for Pd/γ-Al 2O 3, it was ca 52%. The addition of co-catalyst Cu inhibited the decomposition reaction. It was found that there was no positive relationship between the decomposition rate of ethyl nitrite and the reactivity of C 2H 5ONO with CO. According to the product distribution, a relatively reasonable mechanism for the decomposition of ethyl nitrite was proposed, involving the sequential dehydrogenation process.