Cationic Zn-Porphyrin Immobilized in Mesoporous Silicas as Bifunctional Catalyst for CO2 Cycloaddition Reaction under Cocatalyst Free Conditions
Tao, Lin1,3; Liu, Lina1,3; Chen, Jian1,3; Yang, Qihua3; Jayakumar, Sanjeevi2,3; Li, He3; Li, Chunzhi1,3
刊名ACS SUSTAINABLE CHEMISTRY & ENGINEERING
2018-07-01
卷号6期号:7页码:9237-9245
关键词Zinc-porphyrin complex SBA-15 CO2 cycloaddition reaction Bifunctional catalyst Cyclic carbonate
ISSN号2168-0485
DOI10.1021/acssuschemeng.8b01548
通讯作者Yang, Qihua(yangqh@dicp.ac.cn)
英文摘要Immobilization of metalloporphyrin onto a solid support is highly desirable in the chemical industry. Herein, we reported for the first time the efficient immobilization of cationic zincporphyrin complexes on mesoporous SBA-15 by a simple one-pot method by refluxing 5,10,15,20-tetrakis(4-pyridyl)porphyrin zinc(II) (Zn-TPy), SBA-15, and 3-(trimethoxysilyl)propyl bromide in toluene, DMF, NMP, or THF. Studies suggest that solid catalyst with high Zn content, stiochiometric Br-/Zn ratio, and uniform distribution of active sites could be obtained using DMF as the solvent, possibly related to its suitable polarity. The bifunctional solid material with both Lewis acid site and nucleophile acts as an efficient catalyst for catalyzing cycloaddition of CO2 and epoxides under cocatalyst free conditions. Compared with the homogeneous counterpart, the solid catalyst is more active (TOF = 1686 h(-1) versus 370 h-(1)). This suggests that the closely connected Lewis acid and Br in the solid material could enhance their cooperation during the catalytic process. This work provides an efficient method for the synthesis of bifunctional solid catalyst exhibiting enhanced cooperation activation effect for the CO2 cycloaddition reaction.
资助项目National Key R&D Program of China[2017YFB0702800] ; National Natural Science Foundation of China[21733009] ; National Natural Science Foundation of China[21621063] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB17020200] ; International College, University of Chinese Academy of Sciences (UCAS) ; World Academy of Sciences (TWAS)
WOS关键词METAL-ORGANIC FRAMEWORK ; CYCLIC CARBONATES ; HETEROGENEOUS CATALYST ; IONIC LIQUID ; EFFICIENT CYCLOADDITION ; AMBIENT CONDITIONS ; MILD CONDITIONS ; EPOXIDES ; DIOXIDE ; POLYMER
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Engineering
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000444924500127
资助机构National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; International College, University of Chinese Academy of Sciences (UCAS) ; International College, University of Chinese Academy of Sciences (UCAS) ; World Academy of Sciences (TWAS) ; World Academy of Sciences (TWAS) ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; International College, University of Chinese Academy of Sciences (UCAS) ; International College, University of Chinese Academy of Sciences (UCAS) ; World Academy of Sciences (TWAS) ; World Academy of Sciences (TWAS) ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; International College, University of Chinese Academy of Sciences (UCAS) ; International College, University of Chinese Academy of Sciences (UCAS) ; World Academy of Sciences (TWAS) ; World Academy of Sciences (TWAS) ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; International College, University of Chinese Academy of Sciences (UCAS) ; International College, University of Chinese Academy of Sciences (UCAS) ; World Academy of Sciences (TWAS) ; World Academy of Sciences (TWAS)
内容类型期刊论文
源URL[http://cas-ir.dicp.ac.cn/handle/321008/167048]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Yang, Qihua
作者单位1.Univ Chinese Acad Sci, Yuquan Rd 19A, Beijing 100049, Peoples R China
2.Univ Chinese Acad Sci, Int Coll, Yuquan Rd 19A, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, iChEM, 457 Zhongshan Rd, Dalian 116023, Peoples R China
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Tao, Lin,Liu, Lina,Chen, Jian,et al. Cationic Zn-Porphyrin Immobilized in Mesoporous Silicas as Bifunctional Catalyst for CO2 Cycloaddition Reaction under Cocatalyst Free Conditions[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2018,6(7):9237-9245.
APA Tao, Lin.,Liu, Lina.,Chen, Jian.,Yang, Qihua.,Jayakumar, Sanjeevi.,...&Li, Chunzhi.(2018).Cationic Zn-Porphyrin Immobilized in Mesoporous Silicas as Bifunctional Catalyst for CO2 Cycloaddition Reaction under Cocatalyst Free Conditions.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,6(7),9237-9245.
MLA Tao, Lin,et al."Cationic Zn-Porphyrin Immobilized in Mesoporous Silicas as Bifunctional Catalyst for CO2 Cycloaddition Reaction under Cocatalyst Free Conditions".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 6.7(2018):9237-9245.
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