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Efficient synthesis of bio-derived polycarbonates from dimethyl carbonate and isosorbide: regulatingexo-OH andendo-OH reactivity by ionic liquids

文献类型：期刊论文

作者Qian, Wei1,2; Ma, Xifei1,2; Liu, Lei2; Deng, Lili1,2; Su, Qian2; Bai, Ruibing2; Zhang, Zengliang2; Gou, Haibin1,2; Dong, Li2; Cheng, Weiguo2
刊名GREEN CHEMISTRY
出版日期2020-08-21
卷号22期号:16页码:5357-5368
ISSN号1463-9262
DOI10.1039/d0gc01804j
英文摘要It is an immense challenge to design catalysts for synthesizing high molecular weight polycarbonates using CO2, CO2-based compounds, or biorenewable chemicals as building blocks. To this end, an eco-compatible approach to synthesizing polycarbonates from biorenewable isosorbide and CO2-derived dimethyl carbonate (DMC) has been exploited: the regulation of poly(isosorbide carbonate) molecular weight can be achieved by modifying the cation structure of ionic liquid (IL) catalysts. The hydrogen bond donating and accepting ability of ILs can be altered by adjusting the cation structure, which successfully leads to the tunability of the intrinsic imbalance reactivity ofexo-OH andendo-OH in isosorbide. Moreover, these ILs exclusively activate the carbonyl carbon of DMC for accelerating the polymerization reaction. These features are appealing superiorities of ILs as compared to catalysts involving metallic elements. The [Emim]Br catalyst remarkably decreased the imbalanced reactivity of -OH groups of isosorbide, and exhibited the highest catalytic activity. With the presence of [Emim]Br, the poly(isosorbide carbonate) (PIC) weight-average molecular weight and glass transition temperature attained were 52 100 g mol(-1)and 156 degrees C, respectively. Additionally, according to experimental results, DFT calculations, andin situ(1)H NMR analysis, a possible polymerization mechanism indicates that bromine-derived ILs participate in nucleophilic-electrophilic dual-activation in catalyzing PIC synthesis. Our work offers a direction to design catalysts for synthesizing PICs with higher molecular weights through an eco-compatible route.
WOS关键词MOLECULAR-ORBITAL METHODS ; BIODERIVED POLYCARBONATES ; CHEMICAL FIXATION ; BASIS-SET ; CO2 ; CATALYSIS ; DIOXIDE ; WEIGHT ; SALTS ; COPOLYCARBONATES
资助项目National Key R&D Program of China[2016YFB0600903] ; National Natural Science Foundation of China[21890763] ; National Natural Science Foundation of China[21908226] ; Innovation Academy for Green Manufacture, Chinese Academy of Sciences[IAGM-2019-A01]
WOS研究方向Chemistry ; Science & Technology - Other Topics
语种英语
WOS记录号WOS:000560944400013
出版者ROYAL SOC CHEMISTRY
资助机构National Key R&D Program of China ; National Natural Science Foundation of China ; Innovation Academy for Green Manufacture, Chinese Academy of Sciences
源URL[http://ir.ipe.ac.cn/handle/122111/41753]  
专题中国科学院过程工程研究所
通讯作者Cheng, Weiguo
作者单位1.Univ Chinese Acad Sci, Sch Chem Engn, 19A Yuquan Rd, Beijing 100049, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, Innovat Acad Green Manufacture,State Key Lab Mult, Beijing Key Lab Ion Liquids Clean Proc,CAS Key La, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714		 Qian, Wei,Ma, Xifei,Liu, Lei,et al. Efficient synthesis of bio-derived polycarbonates from dimethyl carbonate and isosorbide: regulatingexo-OH andendo-OH reactivity by ionic liquids[J]. GREEN CHEMISTRY,2020,22(16):5357-5368.
APA Qian, Wei.,Ma, Xifei.,Liu, Lei.,Deng, Lili.,Su, Qian.,...&Xu, Fei.(2020).Efficient synthesis of bio-derived polycarbonates from dimethyl carbonate and isosorbide: regulatingexo-OH andendo-OH reactivity by ionic liquids.GREEN CHEMISTRY,22(16),5357-5368.
MLA Qian, Wei,et al."Efficient synthesis of bio-derived polycarbonates from dimethyl carbonate and isosorbide: regulatingexo-OH andendo-OH reactivity by ionic liquids".GREEN CHEMISTRY 22.16(2020):5357-5368.

入库方式： OAI收割

来源：过程工程研究所

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