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利用FT-IR、同位素技术和内循环反应等方法考察了CeO_2和P_6O_11的表面羟基及其与CO反应的活性。CeO_2和Pr_6O_11经高温脱气处理后表面大量的碳酸基和羟基脱附。但部分残留的表面羟基反应活性很高,在200℃甚至更低温度可与CO反应形成表面甲酸基物种,当温度超过300℃时,表面甲酸基物种被表面晶格氧进一步氧化为表面碳酸基物种,但部分表面羟基又复原。认为经高温脱气处理后造成表面配位不饱和中心并使表面羟基得到活化,故易与CO反应形成表面甲酸基。表面甲酸基是CO氧化为CO_2的中间物,表面羟基起活化CO和形成表面甲酸基中间物的作用。
The surface hydroxyl groups of CeO_2 and P_6O_11 and their reactivity with CO were investigated by FT-IR, isotope techniques and internal cyclic reactions. CeO_2 and Pr_6O_11 after degassing at high temperature surface after a large number of carbon-based and hydroxyl desorption. However, some residual surface hydroxyl groups are highly reactive and can react with CO to form surface formic acid-based species even at temperatures below 200 ° C. When the temperature exceeds 300 ° C, the surface formic acid-based species are further oxidized to surface carbonic acid groups by surface lattice oxygen Species, but part of the surface hydroxyl and recovery. It is considered that after the high temperature degassing treatment causes the surface coordination unsaturated center and the surface hydroxyl group to be activated, it is easy to react with CO to form the surface formic acid group. The surface formic acid group is an intermediate for the oxidation of CO to CO 2 and the surface hydroxyl groups act to activate CO and form surface formate based intermediates.