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Titanate nanotube-promoted chemical fixation of carbon dioxide to cyclic carbonate: a combined experimental and computational study
Chen, Aibing1; Zhao, Tiancong1,2; Gao, Hui2; Chen, Limin3; Chen, Jinzhu2; Yua, Yifeng1
2016
Source PublicationCATALYSIS SCIENCE & TECHNOLOGY
Volume6Issue:3Pages:780-790
AbstractTitanate nanotubes (TNT) were found to be air-and water-tolerant, efficient, and recyclable Lewis acid catalysts towards the cycloaddition of carbon dioxide (CO2) to propylene oxide (PO) for the synthesis of cyclic propylene carbonate (PC). Using TNT as the catalyst and potassium iodide, tetrabutylammonium bromide or tetraphenylphosphonium bromide as the co-catalyst, PO was readily converted to PC with a yield of up to >99.9% and a PC selectivity of 100% under relatively mild conditions. Experimental research revealed that the TNT catalyst with the highest exposure of active sites, including surface hydroxyl groups and Lewis acid sites, proved to be the most active for the cycloaddition reaction. Our theoretical evaluation based on density functional theory calculations further indicated that the high Lewis acidity of TNT strongly reduces the energy barrier for the ring-opening step through the polarization of the C-O bond of PO, which allows a subsequent nucleophilic attack easily. Both experimental and computational studies demonstrated that the synergetic effect between TNT and the co-catalyst plays an important role in PC formation. The TNT catalyst is richer in surface Lewis acid sites, shows a large surface area and mesoporous structure, and has a heterogeneous and recyclable nature, which makes TNT an excellent, interesting and ideal catalyst for chemical fixation of CO2.
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1039/c5cy01024a
WOS Subject ExtendedChemistry
WOS KeywordFUNCTIONALIZED IONIC LIQUID ; HIGHLY EFFICIENT CATALYST ; PROPYLENE-OXIDE ; PHOTOCATALYTIC ACTIVITY ; CALCINATION TEMPERATURE ; CHROMIUM PORPHYRIN ; ORGANIC CARBONATES ; BASE CATALYSTS ; CO2 ; EPOXIDES
Indexed BySCI
Language英语
WOS SubjectChemistry, Physical
WOS IDWOS:000369533400022
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Document Type期刊论文
Identifierhttp://ir.giec.ac.cn/handle/344007/11011
Collection中国科学院广州能源研究所
Affiliation1.Hebei Univ Sci & Technol, Coll Chem & Pharmaceut Engn, Shijiazhuang 050018, Peoples R China
2.Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
3.S China Univ Technol, Sch Environm & Energy, Guangzhou Higher Educ Mega Ctr, Guangzhou 510006, Guangdong, Peoples R China
Recommended Citation
GB/T 7714
Chen, Aibing,Zhao, Tiancong,Gao, Hui,et al. Titanate nanotube-promoted chemical fixation of carbon dioxide to cyclic carbonate: a combined experimental and computational study[J]. CATALYSIS SCIENCE & TECHNOLOGY,2016,6(3):780-790.
APA Chen, Aibing,Zhao, Tiancong,Gao, Hui,Chen, Limin,Chen, Jinzhu,&Yua, Yifeng.(2016).Titanate nanotube-promoted chemical fixation of carbon dioxide to cyclic carbonate: a combined experimental and computational study.CATALYSIS SCIENCE & TECHNOLOGY,6(3),780-790.
MLA Chen, Aibing,et al."Titanate nanotube-promoted chemical fixation of carbon dioxide to cyclic carbonate: a combined experimental and computational study".CATALYSIS SCIENCE & TECHNOLOGY 6.3(2016):780-790.
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