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Highly efficient synthesis of novel bio-based pentamethylene dicarbamate via carbonylation of pentanediamine with ethyl carbamate over well-defined titanium oxide catalysts

文献类型：期刊论文

作者Hui, Xiang1,2,3; Wang, Liguo1,2,3,4; Cao, Yan1; Xu, Shuang1; He, Peng1; Li, Huiquan1,2,3,5
刊名CATALYSIS SCIENCE & TECHNOLOGY
出版日期2022-03-02
页码13
ISSN号2044-4753
DOI10.1039/d2cy00073c
英文摘要Carbonylation of pentanediamine (PDA) is a green and effective route for the synthesis of pentamethylene dicarbamate (PDC), an important intermediate compound for the preparation of polyurethanes (PUs) and other chemicals. In this work, TiO2-101 and TiO2-110 catalysts with preferential exposure of (101) and (110) facets, respectively, were prepared and studied for the carbonylation of PDA with ethyl carbamate (EC). The catalysts were characterized by various techniques, including XRD, BET, SEM, TEM, XPS, NH3-TPD, and in situ FTIR. The characterization results indicated that TiO2 catalysts with exposed (110) and (101) facets were synthesized successfully. The overall results suggested that the (101) facets on the TiO2 surface provide high amounts of surface Lewis acid sites that played a pivotal role in PDC formation, which gave a conversion and yield both up to 99% under optimized conditions. In situ FTIR spectroscopy clearly revealed that polyurea as an intermediate was formed in the reaction and subsequently converted to PDC catalyzed by the TiO2 catalyst. Furthermore, the DFT results showed that the conversion of polyurea to PDC over the (101) facets was more prone to occur than the (110) facets due to the lower reaction energy barrier. In addition, the TiO2-101 catalyst displayed excellent stability without an obvious activity decline after five cycles. Furthermore, this strategy also could be successfully expanded to the efficient syntheses of a series of N-substituted carbamates.
WOS关键词PHOSGENE-FREE SYNTHESIS ; N-PHENYL CARBAMATE ; METHYL CARBAMATE ; IONIC LIQUID ; CO2 ; 1,6-HEXAMETHYLENEDIAMINE ; POLYURETHANE ; FACETS ; ROUTE ; ISOCYANATES
资助项目"Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences[XDA 21030600] ; Science and Technology Service Network Initiative, Chinese Academy of Sciences[KFJ-STS-QYZD-138]
WOS研究方向Chemistry
语种英语
出版者ROYAL SOC CHEMISTRY
WOS记录号WOS:000762993500001
资助机构"Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences ; Science and Technology Service Network Initiative, Chinese Academy of Sciences
源URL[http://ir.ipe.ac.cn/handle/122111/52313]  
专题中国科学院过程工程研究所
通讯作者Wang, Liguo
作者单位1.Chinese Acad Sci, Natl Engn Res Ctr Green Recycling Strateg Met Res, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Sino Danish Coll, Beijing 100049, Peoples R China
3.Univ Chinese Acad Sci, Sino Danish Ctr Educ & Res, Beijing 100049, Peoples R China
4.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
5.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714		 Hui, Xiang,Wang, Liguo,Cao, Yan,et al. Highly efficient synthesis of novel bio-based pentamethylene dicarbamate via carbonylation of pentanediamine with ethyl carbamate over well-defined titanium oxide catalysts[J]. CATALYSIS SCIENCE & TECHNOLOGY,2022:13.
APA Hui, Xiang,Wang, Liguo,Cao, Yan,Xu, Shuang,He, Peng,&Li, Huiquan.(2022).Highly efficient synthesis of novel bio-based pentamethylene dicarbamate via carbonylation of pentanediamine with ethyl carbamate over well-defined titanium oxide catalysts.CATALYSIS SCIENCE & TECHNOLOGY,13.
MLA Hui, Xiang,et al."Highly efficient synthesis of novel bio-based pentamethylene dicarbamate via carbonylation of pentanediamine with ethyl carbamate over well-defined titanium oxide catalysts".CATALYSIS SCIENCE & TECHNOLOGY (2022):13.

入库方式： OAI收割

来源：过程工程研究所

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