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The Al(III)-based polydentate chelate complex catalyzed cycloaddition of carbon dioxide and epoxides: synthetic optimization and mechanistic study
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-07-14 , DOI: 10.1039/d2re00196a Hong-Qing Fu 1 , Haifang Mao 1 , Chaoyang Wang 1 , Kun Yin 2 , Miaomiao Jin 1 , Zhenbiao Dong 1 , Yun Zhao 1 , Jibo Liu 1
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2022-07-14 , DOI: 10.1039/d2re00196a Hong-Qing Fu 1 , Haifang Mao 1 , Chaoyang Wang 1 , Kun Yin 2 , Miaomiao Jin 1 , Zhenbiao Dong 1 , Yun Zhao 1 , Jibo Liu 1
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Aimed at greenhouse gas CO2 high value-added utilization, a N,N′-(propane-1,3-diyl)dipicolinamide (PPPA) supported Al(III) metal–organic polydentate chelate complex (Al-PPPA) was designed and used to efficiently catalyze CO2 to cyclic carbonates. The substrate conversion and product selectivity were more than 95% and 98%, respectively, at 120 °C and 2 MPa CO2 without the presence of a co-catalyst. After 5 times of recycling, the substrate conversion was no less than 88%, which indicated the excellent thermal stability and reusability of the catalyst. Simultaneously, the catalyst showed a widely universal range of substrates including olefin chains, phenyl chains, internal epoxides and fluorine-containing epoxides. Furthermore, the plausible mechanism of the CO2 cycloaddition reaction was explored by employing in situ IR technology. The ring opening of PO, CO2 activation and the formation of the final products were examined visually. This work supplies a new route for the theoretical and experimental exploration of new catalyst design and process understanding for efficient greenhouse gas reuse.
中文翻译：
Al(III)基多齿螯合物催化二氧化碳和环氧化物的环加成：合成优化和机理研究
针对温室气体CO 2的高附加值利用，设计并制备了N , N '-(丙烷-1,3-二基)吡啶二甲酰胺(PPPA)负载的Al( III )金属-有机多齿螯合物(Al-PPPA)。用于高效催化CO 2生成环状碳酸酯。在 120 °C 和 2 MPa CO 2条件下，底物转化率和产物选择性分别超过 95% 和 98%在没有助催化剂的情况下。5次循环利用后，底物转化率不低于88%，表明催化剂具有优异的热稳定性和可重复使用性。同时，该催化剂显示出广泛通用的底物范围，包括烯烃链、苯基链、内环氧化物和含氟环氧化物。此外，采用原位红外技术探索了CO 2环加成反应的合理机理。肉眼检查PO的开环、CO 2活化和最终产物的形成。这项工作为高效温室气体再利用的新催化剂设计和工艺理解的理论和实验探索提供了一条新途径。
更新日期：2022-07-14
中文翻译：
Al(III)基多齿螯合物催化二氧化碳和环氧化物的环加成：合成优化和机理研究
针对温室气体CO 2的高附加值利用，设计并制备了N , N '-(丙烷-1,3-二基)吡啶二甲酰胺(PPPA)负载的Al( III )金属-有机多齿螯合物(Al-PPPA)。用于高效催化CO 2生成环状碳酸酯。在 120 °C 和 2 MPa CO 2条件下，底物转化率和产物选择性分别超过 95% 和 98%在没有助催化剂的情况下。5次循环利用后，底物转化率不低于88%，表明催化剂具有优异的热稳定性和可重复使用性。同时，该催化剂显示出广泛通用的底物范围，包括烯烃链、苯基链、内环氧化物和含氟环氧化物。此外，采用原位红外技术探索了CO 2环加成反应的合理机理。肉眼检查PO的开环、CO 2活化和最终产物的形成。这项工作为高效温室气体再利用的新催化剂设计和工艺理解的理论和实验探索提供了一条新途径。
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