Cheng Zhang , Ning Zhou , Shiting Wang , Xiaoxia Yang , Tingyan Peng , Zhifeng Dai , Feiyong Xiang , Yubing Xiong
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引用次数: 0
摘要
将大气中的二氧化碳高效转化为高附加值化学品仍是一项长期挑战。本研究报道了一种新型的三嗪和氨基功能化聚(离子液体)(PILs)制备策略。凭借丰富的氮物种,新开发的 PILs 在二氧化碳转化生产高价值化学品方面具有巨大潜力。系统研究表明,富氮 PILs 可通过分子内多个活性位点的协同作用促进 CO2 与环氧化物的环化反应。在温和的条件下,无需任何助催化剂和溶剂,即可实现优异的转化率和选择性。此外,PIL 多相催化剂可以很容易地回收并重复使用至少多次,而不会明显丧失活性。密度泛函理论计算表明,富氮 PILs 的优异催化活性归因于氢键供体和三嗪环在催化过程中的协同效应。因此,我们的发现为制造多功能异相催化剂提供了一个多功能平台,可用于高效转化二氧化碳。
Triazine- and amino-functionalized poly(ionic liquid) heterogeneous catalyst for efficient CO2 conversion under mild conditions
The efficient conversion of atmospheric CO2 into high value-added chemicals remains a persistent challenge. In this study, a novel strategy for the fabrication of triazine- and amino-functionalized poly(ionic liquid)s (PILs) was reported. By virtue of the rich nitrogen species, the newly-developed PILs possessed great potential in CO2 conversion to produce high-value chemicals. The systematic investigation illustrated that rich-nitrogen PILs could promote the cycloaddition reaction of CO2 and epoxides through the intramolecular synergy of multiple active sites. Excellent conversion and selectivity were achieved under the mild conditions without any co-catalysts and solvents. In addition, PIL heterogeneous catalysts could be easily recovered and reused at least several times without obvious loss in activity. The density functional theory calculation demonstrated that the superior catalytic activity of rich nitrogen PILs was attributed to the synergistic effect of hydrogen bond donor and triazine ring in the catalytic process. Our finding thus presents a versatile platform for fabricating multi-functional heterogeneous catalysts for efficient CO2 conversion.
期刊介绍:
The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials.
The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications.
The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.