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The crucial roles of guest water in a biocompatible coordination network in the catalytic ring-opening polymerization of cyclic esters: a new mechanistic perspective

文献类型：期刊论文

作者Chen, Sheng-Chun1; Zhang, Fei-Hang1; Huang, Kun-Lin2; Tian, Feng1; Zhang, Zhi-Hui1; Zhou, Renxian3; Feng, Xue-Jun1; Zhou, Xiaoying1; He, Ming-Yang1; Gu, Jiande4
刊名CHEMICAL SCIENCE
出版日期2020-03-28
卷号11期号:12页码:3345-3354
ISSN号2041-6520
DOI10.1039/c9sc06024c
文献子类Article
英文摘要The ring-opening polymerization (ROP) of cyclic esters/carbonates is a crucial approach for the synthesis of biocompatible and biodegradable polyesters. Even though numerous efficient ROP catalysts have been well established, their toxicity heavily limits the biomedical applications of polyester products. To solve the toxicity issues relating to ROP catalysts, we report herein a biocompatible coordination network, CZU-1, consisting of Zn-4(mu(4)-O)(COO)(6) secondary building units (SBUs), biomedicine-relevant organic linkers and guest water, which demonstrates high potential for use in the catalytic ROP synthesis of biomedicine-applicable polyesters. Both experimental and computational results reveal that the guest water in CZU-1 plays crucial roles in the activation of the Zn-4(mu(4)-O)(COO)(6) SBUs by generating mu(4)-OH Bronsted acid centers and Zn-OH Lewis acid centers, having a synergistic effect on the catalytic ROP of cyclic esters. Different to the mechanism reported in the literature, we propose a new reaction pathway for the catalytic ROP reaction, which has been confirmed using density functional theory (DFT) calculations, in situ diffuse reflectance IR Fourier transform spectroscopy (DRIFTS), and matrix-assisted laser desorption/ionization time-of-flight mass spectroscopy (MALDI-TOF MS). Additionally, the hydroxyl end groups allow the polyester products to be easily post-modified with different functional moieties to tune their properties for practical applications. We particularly expect that the proposed catalytic ROP mechanism and the developed catalyst design principle will be generally applicable for the controlled synthesis of biomedicine-applicable polymeric materials.
WOS关键词METAL-ORGANIC FRAMEWORKS ; L-LACTIDE ; COMPLEXES ; DESIGN ; HYDROGENATION ; POLYLACTONES ; OXIDATION ; LACTONES ; DISCRETE ; KINETICS
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000528663000023
出版者ROYAL SOC CHEMISTRY
源URL[http://119.78.100.183/handle/2S10ELR8/309416]  
专题新药研究国家重点实验室
通讯作者Gu, Jiande; Chen, Qun; Wu, Chuan-De
作者单位1.Changzhou Univ, Sch Petrochem Engn, Jiangsu Key Lab Adv Catalyt Mat & Technol, Changzhou 213164, Peoples R China;
2.Chongqing Normal Univ, Coll Chem, Chongqing 401331, Peoples R China;
3.Zhejiang Univ, Dept Chem, Hangzhou 310027, Peoples R China;
4.Chinese Acad Sci, Shanghai Inst Mat Med, State Key Lab Drug Res, Drug Design & Discover Ctr, Shanghai 201203, Peoples R China
推荐引用方式
GB/T 7714		 Chen, Sheng-Chun,Zhang, Fei-Hang,Huang, Kun-Lin,et al. The crucial roles of guest water in a biocompatible coordination network in the catalytic ring-opening polymerization of cyclic esters: a new mechanistic perspective[J]. CHEMICAL SCIENCE,2020,11(12):3345-3354.
APA Chen, Sheng-Chun.,Zhang, Fei-Hang.,Huang, Kun-Lin.,Tian, Feng.,Zhang, Zhi-Hui.,...&Wu, Chuan-De.(2020).The crucial roles of guest water in a biocompatible coordination network in the catalytic ring-opening polymerization of cyclic esters: a new mechanistic perspective.CHEMICAL SCIENCE,11(12),3345-3354.
MLA Chen, Sheng-Chun,et al."The crucial roles of guest water in a biocompatible coordination network in the catalytic ring-opening polymerization of cyclic esters: a new mechanistic perspective".CHEMICAL SCIENCE 11.12(2020):3345-3354.

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来源：上海药物研究所

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