Reinforcing supramolecular hyaluronan hydrogels via kinetically interlocking multiple-units strategy

Ruofan Chen; Yujie Li; Yu Jin; Yawei Sun; Zhiyong Zhao; Yun Xu; Jiang-Fei Xu; Yuanchen Dong; Dongsheng Liu

doi:10.1016/j.carbpol.2023.120703

Reinforcing supramolecular hyaluronan hydrogels via kinetically interlocking multiple-units strategy

Carbohydr Polym. 2023 Jun 15:310:120703. doi: 10.1016/j.carbpol.2023.120703. Epub 2023 Feb 18.

Authors

Ruofan Chen¹, Yujie Li¹, Yu Jin², Yawei Sun³, Zhiyong Zhao⁴, Yun Xu⁵, Jiang-Fei Xu⁶, Yuanchen Dong⁷, Dongsheng Liu⁸

Affiliations

¹ Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing 100084, China; Engineering Research Center of Advanced Rare Earth Materials, (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing, 100084 China.
² Department of ophthalmology, Peking Union Medical College Hospital, Beijing 100005, China.
³ State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering, China University of Petroleum (Huadong), Qingdao, 266580, China.
⁴ The State Key Laboratory of Refractories and Metallurgy, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, China. Electronic address: zhaozhiyong@wust.edu.cn.
⁵ Center for Medical Device Evaluation, National Medical Products Administration, Qixiang Road No.50, Haidian District, Beijing 100081, China.
⁶ Key Laboratory of Organic Optoelectronics & Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing 100084, China.
⁷ CAS Key Laboratory of Colloid Interface and Chemical Thermodynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China; University of Chinese Academy of Sciences, Beijing 100049, China. Electronic address: dongyc@iccas.ac.cn.
⁸ Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing 100084, China; Engineering Research Center of Advanced Rare Earth Materials, (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing, 100084 China. Electronic address: liudongsheng@tsinghua.edu.cn.

PMID: 36925240
DOI: 10.1016/j.carbpol.2023.120703

Abstract

Supramolecular hydrogels exhibit promising potential in biological and clinical fields due to their special dynamic properties. However, most existing supramolecular hydrogels suffer from poor mechanical strength, which severely limits their applications. Here in this study, the Kinetically Interlocking Multiple-Units (KIMU) strategy was applied to the hyaluronan networks by introducing different supramolecular interaction motifs in an organized and alternative manner. Our strategy successfully elevated the energy barrier of crosslinker dissociation to 103.0 kJ mol^-1 and increased the storage modulus of hydrogels by 78 % with the intrinsic dynamic properties preserved. It can be expected that this method would bring a convenient and effective route to fabricate novel supramolecular materials with excellent mechanical properties.

Keywords: Host-guest interaction; Hyaluronan; Kinetically interlocking multiple-units (KIMU) effects; Supramolecular hydrogels.