Catalytic conversion of CO2 to cyclic carbonates through multifunctional zinc-modified ZSM-5 zeolite

Catalytic conversion of CO2 to cyclic carbonates through multifunctional zinc-modified ZSM-5 zeolite
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多功能锌改性ZSM-5沸石催化CO2转化为环状碳酸酯

DOI:
10.1002/cjoc.201700573
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发表时间:
2018
影响因子:
5.4
通讯作者:
Zhang Kan
Zhang Kan
中科院分区:
化学2区
文献类型:
--
作者:
Zhao Qing-Ning;Song Qing-Wen;Liu Ping;Zhang Qian-Xia;Gao Jun-Hua;Zhang Kan

文献摘要

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通过廉价的多相催化剂在低压下高效地生产以二氧化碳为基块的精细化学品是一项具有挑战性的工作。在这里,我们首次提出了一种多功能的多相锌修饰的HZSM-5(ZnHZSM-5)催化剂,用于通过将二氧化碳和环氧化物结合到环状碳酸酯中来提高二氧化碳的质量。由于其具有丰富的Lewis酸、Brnsted酸和Lewis碱中心、较大的比表面积和大量的微孔结构等良好的表面性质,使其具有较高的比表面积和丰富的微孔结构,CO2-TPD、TG-MS等表征手段证实了该催化剂具有较好的活性,同时环氧化合物还通过金属中心和氢键被活化。因此,该反应可以很容易地在催化剂界面上进行,并表现出优异的性能,在工业四正丙基溴化铵存在的情况下,目标产品的产率高达99%(以千克计为90%,含0.004摩尔%的锌HZSM-5和0.015摩尔%的nPr4NBr)。
The production of fine chemicals using CO2 as C1 building block through inexpensive heterogeneous catalysts with high efficiency under low.pressure is challenging. Herein we propose for the first time the utilization of a multifunctional heterogeneous zinc‐modified HZSM‐5 (ZnHZSM‐5) catalyst.for upgrading CO2 by incorporation into cyclic carbonates from CO2 and epoxides. Owing to the nice surface properties such as abundant Lewis acid,.Brønsted acid and Lewis base sites, large surface area, and plenty of micropores, CO2 could be concentrated and well activated in ZnHZSM‐5 verified by.CO2‐TPD, TG‐MS, etc. Meanwhile, the epoxides were also activated through metal center and hydrogen bond. Therefore, the reaction can easily assem‐.ble at the catalyst interface and show exceptional performance, affording the aimed products with high yield of up to 99% in the presence of commercial.tetra‐n‐propylammonium bromide (90% in kilogram scale with 0.004 mol% ZnHZSM‐5 and 0.015 mol% nPr4NBr).