| 有序介孔炭负载铜基催化剂Cu/CMK-3用于气相甲醇氧化羰基化反应 |
| Copper Supported Mesoporous Carbon Cu/CMK-3 for Catalytic Oxy-carbonylation of Methanol in Vapor Phase |
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| 摘要: 通过纳米浇铸法合成了有序介孔炭CMK-3，再通过浸渍法制备了Cu/CMK-3催化剂，并将其用于气相甲醇氧化羰基化反应。N2吸附-脱附测试、X射线衍射（XRD）以及透射电镜（TEM）的表征结果表明，Cu/CMK-3具有序介孔结构，活性Cu物种均匀分散于CMK-3的表面及孔道中，粒径为10~20 nm，远小于相同条件下制备的铜/活性炭（Cu/AC）催化剂。固定床反应器的活性评价结果显示450℃下制备的Cu/CMK-3催化活性最高，反应10 h内碳酸二甲酯（DMC）的时空收率（STY）达到286 mg·g-1·h-1，选择性为76%。长周期活性评价结果表明Cu/CMK-3稳定性较相同条件下制备的Cu/AC有大幅提高，50 h内DMC的STY降低了20%，75 h内降低了28%。 |
| 关键词: 非均相催化 负载型催化剂 纳米浇注法 介孔Cu/CMK-3 碳酸二甲酯 甲醇 氧化羰基化 |
| 基金项目: 中央高校基本科研业务费（No.2017XKZD10）资助项目。 |
| Abstract: Ordered mesoporous carbon CMK-3 was synthesized via the nanocasting route, and used to prepare Cu/CMK-3 catalyst for dimethyl carbonate (DMC) synthesis by oxidative carbonylation of methanol in a gas-phase reaction. The effect of activation temperature on the catalyst structure and catalytic performance were investigated. N2 adsorption-desorption, X-ray diffraction (XRD) and transmission electron microscopy (TEM) results revealed that the Cu/CMK-3 catalysts were mesoporous, the active copper species dispersed well in the surface and pore channels of CMK-3, their diameter were between 10~20 nm, far less than that of Cu/activated carbon (Cu/AC). The corresponding catalytic activity in a fixed-bed reactor increased with the activation temperature and the Cu/CMK-3 catalyst prepared at 450℃ exhibited the best catalytic activity. The space time yield (STY) was 286 mg·g-1·h-1 and the selectivity for DMC was 76% in 10 h running. A long periodic test also confirmed a better catalytic stability of Cu/CMK-3 compared to Cu/AC, the STY of DMC declined by 20% after 50 h reaction and 28% after 75 h reaction. |
| Keywords: heterogeneous catalysis supported catalysts nanocasting mesoporous Cu/CMK-3 dimethyl carbonate methanol oxidative carbonylation |
| 投稿时间：2019-11-01 修订日期：2020-01-05 |
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| 王瑞玉,刘亚丽,樊星,魏贤勇.有序介孔炭负载铜基催化剂Cu/CMK-3用于气相甲醇氧化羰基化反应[J].无机化学学报,2020,36(4):769-776. |
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