Novel Carbon Nitride/Metal Oxide Nanocomposites as Efficient and Robust Catalysts for Coupling of CO2 and Epoxides

Novel Carbon Nitride/Metal Oxide Nanocomposites as Efficient and Robust Catalysts for Coupling of CO2 and Epoxides
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新型氮化碳/金属氧化物纳米复合材料作为 CO2 和环氧化物偶联的高效且稳定的催化剂

DOI:
10.1021/acs.iecr.0c05966
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发表时间:
2021-04-14
影响因子:
4.2
通讯作者:
Sun, Jianmin
Sun, Jianmin
中科院分区:
工程技术3区
文献类型:
--
作者:
Gu, Yongqiang;Ping, Ran;Sun, Jianmin

文献摘要

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通过低共熔溶剂(DES)的热解,开发了几种具有路易斯酸碱双功能的环境友好型石墨氮化碳(g-C3N4)基纳米复合材料。它们被用作二氧化碳环加成到环氧化物的多相催化剂。对催化剂的结构和不同的工艺条件进行了优化,并与已报道的多相催化剂进行了催化活性的比较。此外,还检查了催化剂的可重复使用性和对不同环氧化物的适用性。结果表明,2.0Zn@g-C3N4-550与四丁基溴化铵(TBAB)结合,在90℃、1.5 MPa CO2条件下反应3.0 h,能够高效、选择性地将CO2转化为所需产物。此外,催化剂重复使用5次循环后,未观察到明显的失活现象。基于实验结果,最终提出了一种可能的协同催化机制。
Several environmentally benign graphitic carbon nitride (g-C3N4)-based nanocomposites with Lewis acid-base dual functionalities were developed through the pyrolysis of deep-eutectic solvents (DESs). They were used as heterogeneous catalysts for cycloaddition of CO2 to epoxides. The catalysts' structures and different process conditions were optimized, and a comparison of the catalytic activity was made with reported heterogeneous catalysts. Moreover, the catalyst reusability and applicability to different epoxides were examined. The results showed that the 2.0Zn@g-C3N4-550 combining with tetrabutylammonium bromide (TBAB) could efficiently and selectively convert CO2 into the desired products under the conditions of 90 degrees C, 1.5 MPa CO2 for 3.0 h. In addition, no obvious deactivation was observed after the catalyst was reused for five cycles. Based on the experimental results, a possible synergistic catalytic mechanism was finally proposed.