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氧化/还原预处理对cu2o/ac催化甲醇氧化羰基化的影响

, PP. 1245-1251

Keywords: 铜基催化剂,活性炭,预处理,氧化羰基化,碳酸二甲酯,非均相催化

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Abstract:

?将醋酸铜热解制备的cu2o/ac(活性炭)催化剂,在氧化(o2/n2)和还原(h2/n2、co/n2)气氛下进行预处理。350℃下预处理4h,氧化气氛中cu2o完全被氧化为cuo,还原气氛中cu2o被还原为单质铜。经co/n2预处理的催化剂表面cu0分散性好,催化活性显著升高。在常压固定床微型反应装置上测试,在140℃的反应温度下,碳酸二甲酯的时空收率和选择性分别达到了261.9mg/(g·h)和74.7%。反应后,还原气氛(h2/n2、co/n2)预处理的催化剂与cu2o/ac催化剂中铜物种价态组成趋于一致,催化活性亦趋于一致。关联反应前后催化剂表面铜物种的变化和催化活性的差异,可以认为cu0具有较高的初始催化活性,cu2o活性和价态均较为稳定,cuo活性较低。

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