Progress in Stimulus-Responsive Dendritic Gels※

doi:10.6023/A22080363

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (10): 1424-1435.DOI: 10.6023/A22080363 Previous Articles Next Articles

Special Issue: 中国科学院青年创新促进会合辑

Review

刺激响应型树状分子凝胶的研究进展^※

刘志雄^a^,^*(), 初庆凯^a, 冯宇^b^,^*()

a 山西大同大学化学与化工学院大同 037009
b 常州大学材料科学与工程学院常州 213164

投稿日期:2022-08-19 发布日期:2022-09-14
通讯作者: 刘志雄, 冯宇

作者简介:

刘志雄, 理学博士, 山西大同大学副教授, CSCP海洋污损防护技术专业委员会委员, 2014 年于中国科学院化学研究所获得理学博士学位, 2015～2019年在中国科学院宁波材料技术与工程研究所从事博士后研究, 2019年初调动至山西大同大学化学与化工学院工作至今, 主要研究方向包括: (1)高分子智能凝胶材料; (2)表界面功能材料. 主持了国家自然科学青年基金, 中国博士后科学基金特别资助、中国博士后科学基金面上资助, 宁波市“科技创新2025”重大专项等科研攻关项目10余项, 在Chem, Bi-omacromolecules, Chem. Mater.,和 Chem. Eng. J.等国际著名专业杂志发表研究论文30余篇, 授权国家发明专利6项.

初庆凯, 山西大同大学在读硕士研究生, 主要研究方向: 功能化凝胶材料在金属离子检测、吸附领域中的应用研究.

冯宇, 博士, 常州大学材料科学与工程学院教授. 中国科学院青年创新促进会会员、优秀会员. 2010年于中国科学院化学研究所获得理学博士学位, 同年留所工作, 任助理研究员、副研究员, 2016年10月至2018年1月期间在日本北陆先端科学技术大学院大学开展访问研究. 2022年初调动至常州大学材料科学与工程学院工作至今. 主要研究方向包括: (1)功能超分子凝胶; (2)手性功能分子的设计合成、组装及圆偏振发光性能研究; (3)不对称催化. 截至目前, 以项目负责人身份主持国家自然科学基金、中国科学院和中国科学院化学研究所等科研和人才项目10余项. 在Chem. Soc. Rev., Acc. Chem. Res., J. Am. Chem. Soc., Angew. Chem. Int. Ed.等期刊上发表SCI论文50余篇.

^※ 庆祝中国科学院青年创新促进会十年华诞.

基金资助:
国家自然科学基金(21871270); 国家自然科学基金(21472192); 山西大同大学博士启动基金(2019-B-01); 山西大同自然科学项目(2020YGZX011); 中国科学院海洋新材料与应用技术重点实验室开放基金(2021K02)

Progress in Stimulus-Responsive Dendritic Gels^※

Zhixiong Liu^a(), Qingkai Chu^a, Yu Feng^b()

a School of Chemistry and Chemical Engineering, Shanxi Datong University, Datong 037009, China
b School of Materials Science and Engineering, Changzhou University, Changzhou 213164, China

Received:2022-08-19 Published:2022-09-14
Contact: Zhixiong Liu, Yu Feng
About author:
^※ Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
Supported by:
National Natural Science Foundation of China(21871270); National Natural Science Foundation of China(21472192); Doctor Research Fund of Shanxi Datong University(2019-B-01); Science Foundation of Shanxi Datong University(2020YGZX011); Open Research Fund of Key Laboratory of Marine Materials and Related Technologies, CAS(2021K02)

In recent years, stimulus-responsive supramolecular gels, as a class of smart soft matter materials, have shown very promising applications in the fields of ion recognition materials, self-healing materials, biomaterials and drug release, and have attracted increasing attentions. Dendrimers and dendrons are highly branched macromolecules with well-defined molecular architecture and have been widely used as building blocks in the self-assembling of supramolecular gel-phase materials. The unique dendritic architectures make the dendritic molecules as ideal candidates to be modified with various different functional moieties to develop multiple functional soft materials, which ensure each functionality to work independently without interfering. This characteristic makes them show unique advantages in the construction of stimuli- responsive gels, especially multiple stimuli-responsive gels. The research progress of stimuli-responsive dendritic gels is summarized in detail from the aspects of dendritic gel design, gel-formation mechanism, response performance and response mechanism. Based on the different stimulus, the stimulus-responsive dendritic gels are classfied into the following categories: light-responsive dendritic gel, redox-responsive dendritic gel, ion-responsive dendritic gel, thixotropic-responsive dendritic gel and multiple-responsive dendritic gel. In addition, the current challenges and perspectives on stimulus-responsive dendritic gels are also discussed.

Key words: supramolecular gels, dendrimer, stimuli-responsive, smart materials, progress

Cite this article

Zhixiong Liu, Qingkai Chu, Yu Feng. Progress in Stimulus-Responsive Dendritic Gels^※[J]. Acta Chimica Sinica, 2022, 80(10): 1424-1435.

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Fig. & Tab. 24

Figure 1. The structures of first example for dendritic hydrogelator 1 and organogelator 2

Figure 2. (a) The structure of focal azobenzene modified poly(Gly-Asp) dendron 3; (b) schematic diagram of gel-solution transition before and after illumination (ethyl acetate, 0.1% (w))

Figure 3. (a) The chemical structure of asymmetric bis-dendritic gelator 4; photographs of the cyclohexane gel of 4 (0.05% w/V) (b) before and (c) after UV irradiation; the corresponding SEM images from the (d) gel state and (e) solution state

Figure 4. Photographs of the gels and illustration of the reversible phase transitions of (a) dendritic gelator 5 and (b) host-guest inclusion supra- dendron 5/α-CD. The concentration of 5 gelator was 0.41% (w) in both cases, the 5/α-CD molar ratio was 1∶1

Figure 5. (a) The chemical structure of spiropyran-functionalized dendron 6; (b) schematic representation of the self-assembly of dendron 6 into particles and network structure within the organogel, and the corresponding transformations under UV and visible irradiation as well as the corresponding CLSM images

Figure 6. Anthracene and p-nitrocinnamate modified dendritic hydrogelator 7 and organogelator 8

Figure 7. (a) The chemical structures of tetrathiafulvalene (TTF) and monopyrrolotetrathiafulvalene (MPTTF) cored poly(aryl ether) dendron 9~11; (b) the photographs of the two-component dendritic organogels formed by 9/chloranil (30 mg•mL-1, benzene/acetonitrile, 1∶1, V/V): the solution formed after addition of Sc(CF3SO3)3; the recovery of the gel phase after further stirring with magnesium strips, followed by heating and cooling

Figure 8. (a) The chemical structures of ferrocene-based dendron gelators 12 and 13; (b) the photographs of the organogel 12 (4 mg•mL-1, CH3CN/THF) and the formed solution after adding with CAN; (c) the corresponding UV/Visible spectra of the dendritic organogel 12 in presence (red) and absence of CAN (black)

Figure 9. The chemical structure of dendritic ligand 14, and the photographs of the organogel formed by dendritic ligand 14 and silver ions as well as the formed solution upon counteranion exchange

Figure 10. The molecular structures of glycine-glutamic-acid and carbazole-based dendritic gelators 15 and 16

Figure 11. The molecular structures of the naphthalene, anthracene, pyrene cored AB3 type poly(aryl ether) dendritic gelators 17~22

Figure 12. The pictures of organogel formed from 17 in THF (4 mg•mL-1) and after addition of F? (1 equiv.)

Figure 13. (a) The chemical structure of halogen bond donor modified dendritic organogelator 24. (b) Photographs of the dendritic gel 24 in acetone/n-hexane mixed solvent (1∶8, V/V, 12.0 mg•mL-1) before and after the addition of chloride anion. SEM images of (c) the gel state and (d) the aggregate from the sol state after the addition of chloride anion. (e) Calculated structure of the 24-Cl- complex and (f) electrostatic potential surface of 24 (chloride-bound conformation, blue indicates sites of partial positive charge and red sites of partial negative charge)

Figure 14. Schematic representation of bromide anion-responsive of discrete rhomboidal metallacyclic 25~27 gels

Figure 15. The chemical structure of terpyridine attached AB3 type poly(aryl ether) dendron 32

Figure 16. (a) The photographs of the gel-to-solution phase transition of the dendritic gel 12 (4 mg•mL-1) in CH3CN/THF triggered by addition of Pb2+ ion and the recovery of the gel phase after further addition of OAc-; the corresponding SEM images for (b) solution and (c) gel state

Figure 17. The chemical structures of pyridine cored poly(aryl ether) dendrons 33 and 34

Figure 18. The molecular structures of the 3,4-disubstituted twin-dendritic organogelators

Figure 19. (a) Molecular structures of peripherally DMIP-functionalized poly(benzyl ether) dendrons 41 and 42; (b) reversible sol-gel phase transition of the gels of 42 in 1,2-dichloroethane gel (6 mmol•L-1) triggered by external mechanical stress; rheological data of 42 gel from 1,2-dichloroethane (15 ℃, 6 mmol•L-1): (c) strain amplitude sweeps, and (d) time sweep measurement

Figure 20. The molecular structure of azo-functionalized poly(aryl ether) dendritic gelator 43 and reversible sol-gel phase transition of dendritic gelator 43, tuned by multiple stimuli (light, temperature, sonication, and shear stress)

Figure 21. (a) The molecular structure of poly(aryl ether) dendritic gelator 44. (b) Reversible sol-gel phase transition of dendritic gelator 44, tuned by multiple stimuli (temperature, anions, and shear stress)

Figure 22. The molecular structures of poly(aryl ether) dendritic metallogelators 45 and 46

Figure 23. (a) The molecular structure of 2-(2'-hydroxyphenyl) benzoxazole cored poly(aryl ether) dendritic gelator 47. (b) Reversible sol-gel phase transition of dendritic gelator 47 tuned by multiple chemical stimulus (e.g. fluorine ion, zinc ions and pH value) and physical stimulus (e.g. temperature, sonication, and shear stress)

Figure 24. Molecular structures of azobenzene- and quinoline-cored poly(aryl ether) dendritic gelators 48 and 49

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刺激响应型树状分子凝胶的研究进展^※

Progress in Stimulus-Responsive Dendritic Gels^※

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刺激响应型树状分子凝胶的研究进展※

Progress in Stimulus-Responsive Dendritic Gels※

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刺激响应型树状分子凝胶的研究进展^※

Progress in Stimulus-Responsive Dendritic Gels^※