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醋酸铜热解制备无氯Cu2O/AC催化剂及其催化氧化羰基化 被引量:30

Chloride-free Cu_2O/AC Catalyst Prepared by Pyrolysis of Copper Acetate and Catalytic Oxycarbonylation
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摘要 以醋酸铜为前驱物,采用浸渍法负载后进行热处理使醋酸铜热解,获得了负载型无氯Cu2O/AC(活性炭)催化剂,并通过催化甲醇直接气相氧化羰基化合成碳酸二甲酯(DMC).在氮气和惰性气体气氛下,一水合醋酸铜Cu(CH3COO)2·H2O在30~450℃范围内产生3个失重过程,其中在150—300℃范围内Cu(CH3·COO)2热解生成Cu2O;而在300~450℃范围内生成单质Cu.在200~350℃范围内,将Cu(CH3COO)2·H2O/AC加热处理4h后,催化剂上逐步形成了Cu2O,到350℃时,水合醋酸铜几乎全部转化为Cu2O,并有极少量单质Cu形成.在300~350℃热处理4h后,催化剂中铜主要以Cu2O形式存在,并表现出良好的氧化羰基化催化活性.在n(CO):n(MeOH):n(O2)=4:10:1及SV=5600h^-1条件下,于300℃热处理4h所制备的催化剂的甲醇转化率达到6.21%,DMC的时空收率为128.16mg·g^-1·h^-1,选择性为64.26%. The chloride-free Cu2O/AC catalyst was prepared via pyrolysis of copper acetate supported on active carbon Cu (CH3 COO)2/AC and used to catalyze vapor-phase oxycarbonylation of methanol to dimethyl carbonate(DMC). The Cu (CH3COO)2AC precursor was prepared by the incipient wetness impregnation. When Cu(CH3COO)2·H2O was heated from 30 ℃ to 450 ℃ under inert nitrogen atmosphere, it decomposed successively to Cu( CH3COO) 2, Cu2O and Cu, corresponding to three chemical processes. Cu2O was obtained at 150-300 ℃ heating temperature, and Cu was formed at 300-450 ℃. When Cu(CH3COO)2·H2O/AC was heated at 200-350 ℃ for 4 h, Cu2O was gradually formed on the surface of AC. The Cu2O/AC catalyst with predominant Cu2O and only a little Cu was obtained when Cu(CH3COO)2·H2O/AC heated at 350 ℃ for 4 h. It was observed that the Cu2O/AC catalyst heat-treated at 300-350 ℃ for 4 h exhibited very high catalytic activity for methanol oxycarbonylation. On the conditions of n (CO) : n (MeOH) : n ( O2 ) = 4:10:1 and SV = 5600 h^-1, and in the presence of Cu2O/AC catalyst prepared at 300 ℃ for 4 h, the methanol conversion, the space time yield and the selectivity of DMC was reached 6. 21%, 128.16 mg·g^-1· h^-1 and 64.26%, respectively.
出处 《高等学校化学学报》 SCIE EI CAS CSCD 北大核心 2009年第10期2024-2031,共8页 Chemical Journal of Chinese Universities
基金 国家自然科学基金(批准号:20576085) 国家“九七三”计划(批准号:2005CB221204)资助
关键词 醋酸铜 热解 Cu2O/AC催化剂 氧化羰基化 碳酸二甲酯 Copper acetate Pyrolysis Cu2O/AC catalyst Oxycarbonylation Dimethyl carbonate
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